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S  Nϖk_/k_/ _=g  n*@ G ##G G jj  N ۖk_/k_/ _u 1=g   p*@ G ##G G jj  Nk_/k_/ _f5F=g  p*@ G ##G G jjH  0!M ? 3380___PPT10.;Pw poster_Madridg 0 ff l@|f(  N @ C &A darko1E/\f @ 0"`D.cFx  c $dE J   x  c $F _Jd     TG k_/k_/ >""%E     <J |#$& " Tetrachlorosemiquinone anion radical salt of potassium was prepared [1] and crystallised as 2-butanone solvate. Its structural and magnetic characteristics were studied by variable-temperature single crystal X-ray diffraction, DFT (wB97XD) and CAS-MP2 calculations, and magnetic susceptibility measurements in the temperature range from 10-340 K. The X-ray structure analysis detected the two polymorphs at 100 K and 200 K which undergo reversible phase transition in the range 120-170 K. The 100 K-structure reveals -stacked dimers of anion radicals with interplanar separation distance of 3.272 (2) with offset of 1.573 . The infinite stack of dimers repeated by translation reveals interdimer separation distance of 4.353(3) and offset of 2.504 . Diamagnetic response of this crystalline phase involves the antiparallel electron-spin coupling between the two contiguous anion radicals. These dimers continuously uncouple their electron-spins with increasing temperature, which leads to an increase of paramagnetic contribution to magnetisation. The continuous phase transition can be monitored by measuring the unit cell parameters in the range 120-170 K, with a step of 5 K; the volume of monoclinic unit cell of 100 K-polymorph was reduces two times with respect to the 200 K-polymorph. The paramagnetic 200 K-structure is characterised by interplanar separation distance of radical anions of 3.467 and offset of 2.090 . According to the literature [2] solvates and solvent-free crystals reveal different magnetic behaviour, so crystal engineering approach was introduced; to design crystals of desired magnetic properties one can vary the size and polarisability of the cation, and polarity and size of solvent molecule. [3] &$      R  !   v   I     H     1 r8X  0 q  WIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [3] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G G  04l B0IKJ Dimorpism was detected by X-ray structure analysis: 100 K temperature polymorph is caracterised by dimerised radical anion with short intradimer distance and diamagnetic properties, whereas 200 K polymorh reveals stacks of equidistant radical anions with paramagnetic characteristic. The reversible phase transition, structural and magnetic, occurs in the temperature interval 120-170 K.(2 G   0 GD--G P(2  G  " 0 ]n%sGe Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Spin coupling of radical anions detected. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.Pj ('\&H G <  BL$ yM3GLQ VEnergies of the semiquinone radical pairs (in kcal/mol, relative to the lowest value) :V U&  U  \ B  <t<   t  1IJGBR @ #"&k_Q02 IXY a  <\ ?CCPGBR 0.14(fF @  @@`` `  < ?F>PCCBR 0.04(fF @  @@`` _  < ?9PF>BR 4.94(fF @  @@`` ^  < ?5P9BR 4.94(fF @  @@`` ]  < ? 1P5BR LT-L4(fF @  @@`` \  <| ?CC?OGP 0.44(fF @  @@`` [  <@ ?F>?OCCP 0.34(fF @  @@`` Z  < ?9?OF>P 3.64(fF @  @@`` Y  < ?5?O9P 3.44(fF @  @@`` X  < ? 1?O5P HT4(fF @  @@`` W  <$ ?CCMG?O 1.74(fF @  @@`` V  <L ?F>MCC?O 0.84(fF @  @@`` U  <8 ?9MF>?O 2.04(fF @  @@`` T  <p: ?5M9?O 0.04(fF @  @@`` S  <D ? 1M5?O LT-S4(fF @  @@`` R  <pO ?CCKGM triplet4(fF @  @@`` Q  <O ?F>KCCM singlet4(fF @  @@`` P  <Y ?9KF>M triplet4(fF @  @@`` O  <n ?5K9M singlet4(fF @  @@`` N  <0y ? 1K5M ZF  #G j L  <| ?F>IJGK  DFT(wB97XD)4 ( fF @  @@`` J  < ?5IJF>K CAS-MP24(fF @  @@`` I  < ? 1IJ5K ZF  #G jTB b  c $ ? 1IJGIJTB c  c $ ? 1BRGBRTB d  c $ ? 1IJ 1BRTB e  c $ ?GIJGBRTB h  c $ ? 1KGKTB j  c $ ?5IJ5MZB o  s *1 ?F>IJF>BRZB u  s *1 ? 1MGMTB |  c $ ?9K9BRTB   c $ ?CCKCCBRTB   c $ ? 1?OG?OZB   s *1 ?5M5BRTB   c $ ? 1PGPx @ <A ;??$W, ;` @ C 8A K-aceton_pakung#5* @ 0 C-J. \KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties:t ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ < `Cb.E |$Electronic structure characteristics%%( %G  @ 0 dvpDVi [1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] G. Zanotti, A. Del Pra, Acta Cryst. 1980, B36, 313-316 and references therein. [3] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  + i  rE          -                  G  @ Z wA ,? ?5J* , @ 0$ T6 I >In two isostructural salts, KCl4Q" Me2CO [2,3] and RbCl4Q"Me2CO [3], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.l& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ < 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ <$ >bk"V? |3.27 .& G  @ <. 1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <\9 5-07 |3.46 .& G  @ < E 9.2C; |3.46 .& G  @ <Q =032? |3.46 .& G  @ <X] >Rl@ i100 K diamagnetic G  @ <f /-4@2 j200 K paramagnetic G  @ <s /9<31 ]SQUID G  @ <t F!OG iBefore localisation G  @ <{ F&-OG hAfter localisation G J @ C "A NICSDVRB @@ s *Do*O&'lORB @@ s *DoM+,(NRB @@ s *DoU'(=VRB @@ s *DoT,-URB @@ s *DoTZO,ZRB @@ s *DoOU8lORB @@ s *Do*O)*NORB @@ s *DoM))NRB @@ s *DoT)*URB @@ s *Do V*t+1VRB @ s *DoxU,jURB @ s *Do_E+ihERB @@ s *DoYE ,xURB @@ s *DoeElxUD @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`J,oNXB @@ 0D3 H\H @ < R Y S ^aromatic   G  @ <\ H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer1fB  @ < [   F300th anniversary of Ruer Boakovi$$ $G H  0!M ? 33___PPT10i.;Pw+D=' r = @B +Q?zx] \M?{Ji!d<)Bh(XB"eL` f04&&{hcb.R ~w{ի^M~;;ܴ?+^74#R.ˈ;Jp"UnʌJ(&P cŪD|~<"$1mwE'BI=. ؗ$BᬸkKx{|p?߂P{)a^0~ ;.r>ol 2_[Ax9aW(A1! & @SK5A 26BTb R# j v @A@jq R>H @0\@\A@A<@u 3?H @@  3 A }@>  $$ KB  A 2dHp @F<d{Dެ<ձ4M.4fN43Yh߆ans|&L8yp2MONpd!W0%#g"U4߯! 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0AA0 3f@wʚ;ʚ;g4!d!dl2 0p4pA%<4dddd 0P8s <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    g 0 ff l@|f(  N @ C &A darko1E/\f @ 0"`D.cFx  c $dE J   x  c $F _Jd     TG k_/k_/ >""%E     <J |#$& " Tetrachlorosemiquinone anion radical salt of potassium was prepared [1] and crystallised as 2-butanone solvate. Its structural and magnetic characteristics were studied by variable-temperature single crystal X-ray diffraction, DFT (wB97XD) and CAS-MP2 calculations, and magnetic susceptibility measurements in the temperature range from 10-340 K. The X-ray structure analysis detected the two polymorphs at 100 K and 200 K which undergo reversible phase transition in the range 120-170 K. The 100 K-structure reveals -stacked dimers of anion radicals with interplanar separation distance of 3.272 (2) with offset of 1.573 . The infinite stack of dimers repeated by translation reveals interdimer separation distance of 4.353(3) and offset of 2.504 . Diamagnetic response of this crystalline phase involves the antiparallel electron-spin coupling between the two contiguous anion radicals. These dimers continuously uncouple their electron-spins with increasing temperature, which leads to an increase of paramagnetic contribution to magnetisation. The continuous phase transition can be monitored by measuring the unit cell parameters in the range 120-170 K, with a step of 5 K; the volume of monoclinic unit cell of 100 K-polymorph was reduces two times with respect to the 200 K-polymorph. The paramagnetic 200 K-structure is characterised by interplanar separation distance of radical anions of 3.467 and offset of 2.090 . According to the literature [2] solvates and solvent-free crystals reveal different magnetic behaviour, so crystal engineering approach was introduced; to design crystals of desired magnetic properties one can vary the size and polarisability of the cation, and polarity and size of solvent molecule. [3] &$      R  !   v   I     H     1 r8X  0 q  WIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for  !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~                           ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~        !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~5     r46789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnqstuvwxy{|}~Root EntrydO)0H }p@Pictures(Current User eSummaryInformation( PowerPoint Document(d DocumentSummaryInformation8 Graph Origin50.Graph0Origin Graph;  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin Graphd/ 0DArialNew RomanPP\sؖ2 0ؖ"DTimes New RomanPP\sؖ2 0ؖ B.G  @n?" dd@  @@`` ,$Hr2$#JAQpݸdyq$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74db$r?bL6S!Q!A2$0{r}G^C_`! 0AA0 3f@wʚ;ʚ;g4!d!dl2 0p4pA%<4dddd 0P8s <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    g 0 ff l@|f(  N @ C &A darko1E/\f @ 0"`D.cFx  c $dE J   x  c $F _Jd     TG k_/k_/ >""%E     <J |#$& " Tetrachlorosemiquinone anion radical salt of potassium was prepared [1] and crystallised as 2-butanone solvate. Its structural and magnetic characteristics were studied by variable-temperature single crystal X-ray diffraction, DFT (wB97XD) and CAS-MP2 calculations, and magnetic susceptibility measurements in the temperature range from 10-340 K. The X-ray structure analysis detected the two polymorphs at 100 K and 200 K which undergo reversible phase transition in the range 120-170 K. The 100 K-structure reveals -stacked dimers of anion radicals with interplanar separation distance of 3.272 (2) with offset of 1.573 . The infinite stack of dimers repeated by translation reveals interdimer separation distance of 4.353(3) and offset of 2.504 . Diamagnetic response of this crystalline phase involves the antiparallel electron-spin coupling between the two contiguous anion radicals. These dimers continuously uncouple their electron-spins with increasing temperature, which leads to an increase of paramagnetic contribution to magnetisation. The continuous phase transition can be monitored by measuring the unit cell parameters in the range 120-170 K, with a step of 5 K; the volume of monoclinic unit cell of 100 K-polymorph was reduces two times with respect to the 200 K-polymorph. The paramagnetic 200 K-structure is characterised by interplanar separation distance of radical anions of 3.467 and offset of 2.090 . According to the literature [2] solvates and solvent-free crystals reveal different magnetic behaviour, so crystal engineering approach was introduced; to design crystals of desired magnetic properties one can vary the size and polarisability of the cation, and polarity and size of solvent molecule. [3] &$      R  !   v   I     H     1 r8X  0 q  WIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [3] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G G  04l B0IKJ Dimorpism was detected by X-ray structure analysis: 100 K temperature polymorph is caracterised by dimerised radical anion with short intradimer distance and diamagnetic properties, whereas 200 K polymorh reveals stacks of equidistant radical anions with paramagnetic characteristic. The reversible phase transition, structural and magnetic, occurs in the temperature interval 120-170 K.(2 G   0 GD--G P(2  G  " 0 ]n%sGe Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Spin coupling of radical anions detected. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.Pj ('\&H G <  BL$ yM3GLQ VEnergies of the semiquinone radical pairs (in kcal/mol, relative to the lowest value) :V U&  U  \ B  <t<   t  1IJGBR @ #"&k_Q02 IXY a  <\ ?CCPGBR 0.14(fF @  @@`` `  < ?F>PCCBR 0.04(fF @  @@`` _  < ?9PF>BR 4.94(fF @  @@`` ^  < ?5P9BR 4.94(fF @  @@`` ]  < ? 1P5BR LT-L4(fF @  @@`` \  <| ?CC?OGP 0.44(fF @  @@`` [  <@ ?F>?OCCP 0.34(fF @  @@`` Z  < ?9?OF>P 3.64(fF @  @@`` Y  < ?5?O9P 3.44(fF @  @@`` X  < ? 1?O5P HT4(fF @  @@`` W  <$ ?CCMG?O 1.74(fF @  @@`` V  <L ?F>MCC?O 0.84(fF @  @@`` U  <8 ?9MF>?O 2.04(fF @  @@`` T  <p: ?5M9?O 0.04(fF @  @@`` S  <D ? 1M5?O LT-S4(fF @  @@`` R  <pO ?CCKGM triplet4(fF @  @@`` Q  <O ?F>KCCM singlet4(fF @  @@`` P  <Y ?9KF>M triplet4(fF @  @@`` O  <n ?5K9M singlet4(fF @  @@`` N  <0y ? 1K5M ZF  #G j L  <| ?F>IJGK  DFT(wB97XD)4 ( fF @  @@`` J  < ?5IJF>K CAS-MP24(fF @  @@`` I  < ? 1IJ5K ZF  #G jTB b  c $ ? 1IJGIJTB c  c $ ? 1BRGBRTB d  c $ ? 1IJ 1BRTB e  c $ ?GIJGBRTB h  c $ ? 1KGKTB j  c $ ?5IJ5MZB o  s *1 ?F>IJF>BRZB u  s *1 ? 1MGMTB |  c $ ?9K9BRTB   c $ ?CCKCCBRTB   c $ ? 1?OG?OZB   s *1 ?5M5BRTB   c $ ? 1PGPx @ <A ;??$W, ;` @ C 8A K-aceton_pakung#5* @ 0 C-J. \KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties:t ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ < `Cb.E |$Electronic structure characteristics%%( %G  @ 0 dvpDVi [1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] G. Zanotti, A. Del Pra, Acta Cryst. 1980, B36, 313-316 and references therein. [3] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  + i  rE          -                  G  @ Z wA ,? ?5J* , @ 0$ T6 I >In two isostructural salts, KCl4Q" Me2CO [2,3] and RbCl4Q"Me2CO [3], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.l& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ < 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ <$ >bk"V? |3.27 .& G  @ <. 1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <\9 5-07 |3.46 .& G  @ < E 9.2C; |3.46 .& G  @ <Q =032? |3.46 .& G  @ <X] >Rl@ i100 K diamagnetic G  @ <f /-4@2 j200 K paramagnetic G  @ <s /9<31 ]SQUID G  @ <t F!OG iBefore localisation G  @ <{ F&-OG hAfter localisation G J @ C "A NICSDVRB @@ s *Do*O&'lORB @@ s *DoM+,(NRB @@ s *DoU'(=VRB @@ s *DoT,-URB @@ s *DoTZO,ZRB @@ s *DoOU8lORB @@ s *Do*O)*NORB @@ s *DoM))NRB @@ s *DoT)*URB @@ s *Do V*t+1VRB @ s *DoxU,jURB @ s *Do_E+ihERB @@ s *DoYE ,xURB @@ s *DoeElxUD @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`J,oNXB @@ 0D3 H\H @ < R Y S ^aromatic   G  @ <\ H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer1fB  @ < [   F300th anniversary of Ruer Boakovi$$ $G H  0!M ? 33___PPT10i.;Pw+D='  = @B +rƛ  1 (JV ՜.+,0`    CustomIRBd /' ArialTimes New RomanBookman Old Styleposter_Madrid Origin GraphISIS/Draw Sketch_π-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES  Fonts UsedDesign TemplateEmbedded OLE Servers Slide/_@ |Institut Ruder BokovicInstitut Ruder Boakovic Titles neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [3] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G G  04l B0IKJ Dimorpism was detected by X-ray structure analysis: 100 K temperature polymorph is caracterised by dimerised radical anion with short intradimer distance and diamagnetic properties, whereas 200 K polymorh reveals stacks of equidistant radical anions with paramagnetic characteristic. The reversible phase transition, structural and magnetic, occurs in the temperature interval 120-170 K.(2 G   0 GD--G P(2  G  " 0 ]n%sGe Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Spin coupling of radical anions detected. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.Pj ('\&H G <  BL$ yM3GLQ VEnergies of the semiquinone radical pairs (in kcal/mol, relative to the lowest value) :V U&  U  \ B  <t<   t  1IJGBR @ #"&k_Q02 IXY a  <\ ?CCPGBR 0.14(fF @  @@`` `  < ?F>PCCBR 0.04(fF @  @@`` _  < ?9PF>BR 4.94(fF @  @@`` ^  < ?5P9BR 4.94(fF ,@  @@`` ]  < ? 1P5BR LT-L4(fF @  @@`` \  <| ?CC?OGP 0.44(fF @  @@`` [  <@ ?F>?OCCP 0.34(fF @  @@`` Z  < ?9?OF>P 3.64(fF @  @@`` Y  < ?5?O9P 3.44(fF @  @@`` X  < ? 1?O5P HT4(fF @  @@`` W  <$ ?CCMG?O 1.74(fF @  @@`` V  <L ?F>MCC?O 0.84(fF @  @@`` U  <8 ?9MF>?O 2.04(fF @  @@`` T  <p: ?5M9?O 0.04(fF @  @@`` S  <D ? 1M5?O LT-S4(fF @  @@`` R  <pO ?CCKGM triplet4(fF @  @@`` Q  <O ?F>KCCM singlet4(fF @  @@`` P  <Y ?9KF>M triplet4(fF @  @@`` O  <n ?5K9M singlet4(fF @  @@`` N  <0y ? 1K5M ZF  #G j L  <| ?F>IJGK  DFT(wB97XD)4 ( fF @  @@`` J  < ?5IJF>K CAS-MP24(fF @  @@`` I  < ? 1IJ5K ZF  #G jTB b  c $ ? 1IJGIJTB c  c $ ? 1BRGBRTB d  c $ ? 1IJ 1BRTB e  c $ ?GIJGBRTB h  c $ ? 1KGKTB j  c $ ?5IJ5MZB o  s *1 ?F>IJF>BRZB u  s *1 ? 1MGMTB |  c $ ?9K9BRTB   c $ ?CCKCCBRTB   c $ ? 1?OG?OZB   s *1 ?5M5BRTB   c $ ? 1PGPx @ <A ;??$W, ;` @ C 8A K-aceton_pakung#5* @ 0 C-J. \KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties:t ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ < `Cb.E |$Electronic structure characteristics%%( %G  @ 0 dvpDVi [1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] G. Zanotti, A. Del Pra, Acta Cryst. 1980, B36, 313-316 and references therein. [3] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  + i  rE          -                  G  @ Z wA ,? ?5J* , @ 0$ T6 I >In two isostructural salts, KCl4Q" Me2CO [2,3] and RbCl4Q"Me2CO [3], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.l& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ < 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ <$ >bk"V? |3.27 .& G  @ <. 1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <\9 5-07 |3.46 .& G  @ < E 9.2C; |3.46 .& G  @ <Q =032? |3.46 .& G  @ <X] >Rl@ i100 K diamagnetic G  @ <f /-4@2 j200 K paramagnetic G  @ <s /9<31 ]SQUID G  @ <t F!OG iBefore localisation G  @ <{ F&-OG hAfter localisation G J @ C "A NICSDVRB @@ s *Do*O&'lORB @@ s *DoM+,(NRB @@ s *DoU'(=VRB @@ s *DoT,-URB @@ s *DoTZO,ZRB @@ s *DoOU8lORB @@ s *Do*O)*NORB @@ s *DoM))NRB @@ s *DoT)*URB @@ s *Do V*t+1VRB @ s *DoxU,jURB @ s *Do_E+ihERB @@ s *DoYE ,xURB @@ s *DoeElxUD @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`J,oNXB @@ 0D3 H\H @ < R Y S ^aromatic   G  @ <\ H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <  Hd  F300th anniversary of Ruer Boakovi$$ $G H  0!M ? 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The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0[ rU2 I;a  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0 Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B  <t<   x @ <A E??$W, E` @ C 8A K-aceton_pakung#5, @ 0ܝ C-J. ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ 08 fCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ? 5J, , @ 0 h6 I :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. 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The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0[ rU3SI;a  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0 Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B  <t<   x @ <A E??XB8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ 08 fCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ?4pJ( , @ 0 h\.xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ <X 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ < >bk"V? |3.27 .& G  @ <  1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <) 5-07 |3.46 .& G  @ <4 9.2C; |3.46 .& G  @ <@ =032? |3.46 .& G  @ <DM >Rl@ i100 K diamagnetic G  @ <V /-4@2 j200 K paramagnetic G  @ <c /9<31 ]SQUID G 8 DV A`C029I*UR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <  RY S ^aromatic   G  @ < H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <  Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1EIe A 0_ x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0w `CE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A <T 6@D7 _heating  G   A <\ 68@D9 _cooling 33 G   A <t ;>nI.= nReversible transition!  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ImMxhۜV.O_Kԍhvܢe<:3d}vI9/m(FJ}zįr%Mۗ6/.ûbd/&495_,_)0P`a7le(lx%cR?8B2uGӍt#mm/䢉YkpfYw HI5=f7.[wv{DĂ%xL̤&a >pbV?j&#u]95^_ B,9{Oe=bHQ#zPA^X#{GѻW}J 0O[ QVDS8J>-XZ-nxyIw-ߛXt* tJhxx(2QHI5=fxxhkd"h_4zhh5dW+M z{)ޔm$|vݬs?ŵblE7ۘV;LRxk6ih~K4\u>Ϥ`r#ݨL/I_]Hv]!{: 8|tنyQ9D(S%+w~5G7{tpMDEz9HC>/.t/T=]8ӥeqOzcPbG<[KݤYM7e)RƧ;nD]tG,yfnv m,sp`Ӕ{NdyX KSZSmeKqѦ\{ ,rzk/ݷoo+cct\g[ޒfp%\@< d13 K@< 2 +@ Z /^Y OW@^%* y dFA&[ A ;;p.D+=AOB3A9LmG@)(ȿA|oApA ?ǒ}Zn]@ec}x+vRS?)r$r   ! rT 1;(JVi   E Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hf*b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Z 0 YY `)A0 WY(  x  c $2 J   x  c $2 _Jd     T4 k_/k_/ >""%E     <7 H, R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0[ rU3SI;a  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0 Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B  <t<   x @ <A E??'F^. E` @ C 8A K-aceton_pakungh+, @ 0ܝ C-J. ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ 08 fCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ?4pJ( , @ 0 h\.xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ <X 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ < >bk"V? |3.27 .& G  @ <  1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <) 5-07 |3.46 .& G  @ <4 9.2C; |3.46 .& G  @ <@ =032? |3.46 .& G  @ <DM >Rl@ i100 K diamagnetic G  @ <V /-4@2 j200 K paramagnetic G  @ <c /9<31 ]SQUID G 8 DV A`C029I*UR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <  RY S ^aromatic   G  @ < H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <  Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1EIe A 0_ x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0w `CE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A <T 6@D7 _heating  G   A <\ 68@D9 _cooling 33 G   A <t ;>nI.= nReversible transition!  G L Q4KQI1Z A# SE0U @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A B H(,J _heating  G   A BF J(,kL _cooling 33 G   A Bȥ O#)P jCrystals decompose  G  A <F l]x ^ kEquidistant anions:  G 8 V')e AV)e| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <D +Y!rZ |3.23 .& G  A < #Ha&b |3.23 .& G  A < !]$^ |3.23 .& G L 8 cFR. 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ImMxhۜV.O_Kԍhvܢe<:3d}vI9/m(FJ}zįr%Mۗ6/.ûbd/&495_,_)0P`a7le(lx%cR?8B2uGӍt#mm/䢉YkpfYw HI5=f7.[wv{DĂ%xL̤&a >pbV?j&#u]95^_ B,9{Oe=bHQ#zPA^X#{GѻW}J 0O[ QVDS8J>-XZ-nxyIw-ߛXt* tJhxx(2QHI5=fxxhkd"h_4zhh5dW+M z{)ޔm$|vݬs?ŵblE7ۘV;LRxk6ih~K4\u>Ϥ`r#ݨL/I_]Hv]!{: 8|tنyQ9D(S%+w~5G7{tpMDEz9HC>/.t/T=]8ӥeqOzcPbG<[KݤYM7e)RƧ;nD]tG,yfnv m,sp`Ӕ{NdyX KSZSmeKqѦ\{ ,rzk/ݷoo+cct\g[ޒfp%\@< d13 K@< 2 +@ Z /^Y OW@^%* y dFA&[ A ;;p.D+=AOB3A9LmG@)(ȿA|oApA ?ǒ}Zn]@ec}x+vRS?)r$ ULc    T6 1;(JVi   E Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hf*b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Z 0 YY `)A0 WY(  x  c $2 J   x  c $2 _Jd     T4 k_/k_/ >""%E     <7 H, R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0[ rU3SI;a  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0 Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B  <t<   ` @ C 8A K-aceton_pakungh+, @ 0ܝ C-J. ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepc/>B8 ! ;9IJ @c/o3,Bj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?c/3J@ r @ S JA ,800px-Loligo_vulgaris0(8?6 @ 08 fCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ?4pJ( , @ 0 h\.xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 7"'7XB @ 0D 8"'8^B @ 6D =""9@^B @ 6D "9x x S<^B @ 6D 4  8^B @ 6D 0HH-4 @ <X 12 |3.58 .& G  @ < 9 ; |3.58 .& G  @ < 5/7 |3.27 .& G  @ < >bk"V? |3.27 .& G  @ <  1+#.2 |3.46 .& G ^B @ 6D 0**3^B @ 6D 4,,8^B @ 6D 8x.x.%<^B @ 6D ==0=09@ @ <) 5-07 |3.46 .& G  @ <4 9.2C; |3.46 .& G  @ <@ =032? |3.46 .& G  @ <DM >Rl@ i100 K diamagnetic G  @ <V /-4@2 j200 K paramagnetic G  @ <c /9<31 ]SQUID G 8 DV A`C029I*UR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <  RY S ^aromatic   G  @ < H@ I ]quinoid G  @ < LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <  Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1EIe A 0_ x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0w `CE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A <T 6@D7 _heating  G   A <\ 68@D9 _cooling 33 G   A <t ;>nI.= nReversible transition!  G L Q4KQI1Z A# SE0U @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A B H(,J _heating  G   A BF J(,kL _cooling 33 G   A Bȥ O#)P jCrystals decompose  G  A <F l]x ^ kEquidistant anions:  G 8 V')e AV)e| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <D +Y!rZ |3.23 .& G  A < #Ha&b |3.23 .& G  A < !]$^ |3.23 .& G L 8 cFR. 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ImMxhۜV.O_Kԍhvܢe<:3d}vI9/m(FJ}zįr%Mۗ6/.ûbd/&495_,_)0P`a7le(lx%cR?8B2uGӍt#mm/䢉YkpfYw HI5=f7.[wv{DĂ%xL̤&a >pbV?j&#u]95^_ B,9{Oe=bHQ#zPA^X#{GѻW}J 0O[ QVDS8J>-XZ-nxyIw-ߛXt* tJhxx(2QHI5=fxxhkd"h_4zhh5dW+M z{)ޔm$|vݬs?ŵblE7ۘV;LRxk6ih~K4\u>Ϥ`r#ݨL/I_]Hv]!{: 8|tنyQ9D(S%+w~5G7{tpMDEz9HC>/.t/T=]8ӥeqOzcPbG<[KݤYM7e)RƧ;nD]tG,yfnv m,sp`Ӕ{NdyX KSZSmeKqѦ\{ ,rzk/ݷoo+cct\g[ޒfp%\@< d13 K@< 2 +@ Z /^Y OW@^%* y dFA&[ A ;;p.D+=AOB3A9LmG@)(ȿA|oApA ?ǒ}Zn]@ec}x+vRS?)r$J7E Y J &7; 1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hf*b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Z 0 YY `)A0 WY(  x  c $l<J  x  c $8=_Jd    T>k_/k_/ >""%E        !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{}~   <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakunghU+g- @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?j03JA r @ S JA ,800px-Loligo_vulgaris1(8?7 @ 0LfCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN09<:2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D8 _heating  G   A <=9@D: _cooling 33 G   A <|<>nI5> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G L 8 cFR. (AUD(q6-l A c <AKCl4Q-stackcFR.fB A 6DԔM(M*fB A 6DԔ3L#3L%fB A 6DԔIIr  A <IL t3.50 4Gg  A <L2$N% t3.50 4Gg  A 0xCNr)QP+ t3.50 4Gg fB A 6DԔ3O+3O2-fB A 6DԔLr&L'fB A 6DԔJ2!J" A <tO,Q, t3.10 4Gg  A <8%SM&nO' t3.10 4Gg   A <)Kb!.MG" t3.10 4Gg `B !A 0D SM'SM(`B "A 0D KR"KB#`B #A 0D O-O-`B $A 0D O"+O,`B %A 0D SM%SM&`B &A 0D K K!x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A E??f2F EH  0!M ? 33___PPT10i.;Pw+D=' A= @B +r' g 1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hf*b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    rւ  1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0Pp4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Y 0 XX ^+APeX(  x  c $l<J  x  c $8=_Jd    T>k_/k_/ >""%E     <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakunghU+g- @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?j03JA r @ S JA ,800px-Loligo_vulgaris1(8?7 @ 0LfCi >T[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 5, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN09<:2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D8 _heating  G   A <=9@D: _cooling 33 G   A <|<>nI5> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A E??f2F EH  0!M ? 33___PPT10i.;Pw+D=' A= @B +rM )r 1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    r  1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Y 0 XX ^+APgX(  x  c $l<J  x  c $8=_Jd    T>k_/k_/ >""%E     <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakunghU+g- @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?j03JA r @ S JA ,800px-Loligo_vulgaris1(8?7 @ 0LfCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN09<:2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D8 _heating  G   A <=9@D: _cooling 33 G   A <|<>nI5> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A E??f2F EH  0!M ? 33___PPT10i.;Pw+D=' = @B +r%h Lp 1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 00 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Y 0 XX ^+APgX(  x  c $l<J  x  c $8=_Jd    T>k_/k_/ >""%E     <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakunghU+g- @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0LfCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xI :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0x Bz DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D9 _heating  G   A <9@D2; _cooling 33 G   A <|P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A E??f2F EH  0!M ? 33___PPT10i.;Pw+D=' = @B +rp~ dp 1;(JVi   J Graph Origin50.Graph0Origin GraphE  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!$R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d2$Pwu?d1h"2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0Hp4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Y 0 XX ^+APgX(  x  c $l<J  x  c $8=OJT     T>k_/k_/ >""%E     <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakung+U+*, @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0LfCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0 E<= DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D9 _heating  G   A <9@D2; _cooling 33 G   A <|P=>8I>      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{}~nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A E??Q0)H EH  0!M ? 33___PPT10i.;Pw+D=' = @B +r. A 1;(JVi   L Graph Origin50.GI;9oI%jbBA;baU32u3,33L#4))C>OkSm*ֺmiΎ.c\e?(c\vt)B;F{:c^l53OӸkG?dUNτ-{p>~{ŕ{OG6JK;k"WZW;+Zl<ٯ s?~dǐCvqd'@6l Ad%d%d'D6l0ad#F"Ev )dF6lL0fWtg,B::X*\x*\fRU+YVA%nv~_Eyvf.tǡk'~o_Yk,stJP=hli򇓈Ў.z:m+F]}li>kЎў&<OIifqê>xZtxa )vǝL7~M^Av4idW]Ev 5dב]Gv d7Dv -d3f"E6lx{} Ѷ :_7}B,7YHh)C*d3QUR-53O开]HyJeng u&M_Sg:y^xyo11W<%RO)Ř|oyV=tcVZ{o4eH][k<;d,0hDA;my7]e~{\.Tm62/H?.Ryr>8v]kُ<VۏZqKcߏxM>D?T/ͳ- aXwZ鬳QvAzMz6g{._y}8@#؃]VCa/wV/8,ܪwYZ|00tX,zs/*bAz}]raph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Hd,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4dddd$2 0H-p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    Y 0 XX ^+APgX(  x  c $l<J  x  c $8=OJT     T>k_/k_/ >""%E     <@. R A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtMeCO which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. F !(        > ?       E    @   :  "    U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakung+U+*, @ 08J.J0 ~KCl4Q"MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic properties\t(( ((f( tG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0LfCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY :In two isostructural salts, KCl4Q" Me2CO [2] and RbCl4Q"Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.j& &  .  &  .  &  . / & X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0 E<= DdKCl4Q"Me2CO and RbCl4Q"Me2CO: diamagnetic crystals3(((( ((((( 3G < A 0C6_uE @NH4Cl4Q"MeCN: 1D antiferromagnet`!((((( !G  A < 7@D9 _heating  G   A <9@D2; _cooling 33 G   A <|P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B + bx[klT>ݵ޵1qQ il6)ID#Յ P4!Vm%R*BZU-%Bgx? zwwy;x~w33g<}?UtL>Qj>*v@R]X hV0BTsbW~GYeПa$Wj6U ')&)XHT۳Rg"BC34"VuЀ=VTlJOSr˟/,PJK͓~UJD,ɃDyH@l`RZIwn)'>1zE`v&ͧ U|}B*C*G*F#F!ݏ4i XqH& g1Ф _mOX dHu :ÑdILo ME&4p֟dI?&7zh~V_V?WFXcZ!T|b3S$~;@oXW?\`/rd ֥ ͉*uEa[0g­ kBnl[$;ol]j~T&ap}%ku/2x*>L7F@dP!ʍqۄ̓VH s^Wn {L$_"ZjFnDtѐK '(rPJZn%-JVR \Pxe-pAqܒvyl! 9x<-XyU*SF o;>SS`8 gefx^s#23IDLM" S kt4/SC1ˊ{Nv̋wM&CUW)cu} C&FvR>L#M[gQa4:S|O"sLqp*Kx^{$(&s<ՑkxW(AIq%= .<ǙRʄH|(rWM"2597ޫ|}Ÿڔ2O \-7l6q4ڶ}3y&7%[rBf'cU[2> JనZ by8>yHdQK$'5qC~*og~gqKoۤ>#efuY;zN[wJ Md~, )藪EW+%R[m\fdk>;r4Gmf{2'[` Ѹ2ɛl* БG=۽_n;[&}n~z?{mO]Yl^戴P#1~l>6vz؄&чa]9C~^ֿN}kn5&˼=_=HB4 A*jcDObco $IJvlީv}YM)DBDwt,'ꛟ jXlX&FKcNpݟ_'׉u-2v_'׉{ûE?_;Kz(-wfê$Ĥ"xO";oI ]1l-'oktY4@qS݁WnV^wy1w=K~ݒ/<[v18NL"(S@1/%Nwru5Gg~̎\+%8ߙ&};Nw|o'ۉNo^Ɖvyl'71;d:NmɌVoV3G:Q8ׇLܛou;}SrNAO u *A3 1C(JVi   L Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    H\ 0 _[W[ ^+APZ(  x  c $l<J  x  c $8=OJT     T>k_/k_/ >""%E   x  <@.  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0j>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0,Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ BpC=t=   ` @ C 8A K-aceton_pakung+U+*, @ 08J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0LfCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <H23 |3.58 .& G  @ <: &< |3.58 .& G  @ <668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ < 2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <6-0 8 |3.46 .& G  @ <8;.2J< |3.46 .& G  @ <T*>039@ |3.46 .& G  @ <5?RsA i100 K diamagnetic G  @ <$@0-4G3 j200 K paramagnetic G  @ <LN{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <lL RY S ^aromatic   G  @ <dH@ I ]quinoid G  @ <,lLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ <T{ Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0 E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A < 7@D9 _heating  G   A <9@D2; _cooling 33 G   A <|P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BpK(,!M _cooling 33 G   A BPjO#)P jCrystals decompose  G  A <|^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <+Y!rZ |3.23 .& G  A <H#Ha&b |3.23 .& G  A <!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6x1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A Bt3*5+ t3.10 4Gg  A B8%]0$2% t3.10 4Gg   A B)-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B + bx[klT>ݵ޵1qQ il6)ID#Յ P4!Vm%R*BZU-%Bgx? zwwy;x~w33g<}?UtL>Qj>*v@R]X hV0BTsbW~GYeПa$Wj6U ')&)XHT۳Rg"BC34"VuЀ=VTlJOSr˟/,PJK͓~UJD,ɃDyH@l`RZIwn)'>1zE`v&ͧ U|}B*C*G*F#F!ݏ4i XqH& g1Ф _mOX dHu :ÑdI݁Lo ME&4p֟dI?&7zh~V_V?WFXcZ!T|b3S$~;@oXW?\`/rd ֥ ͉*uEa[0g­ kBnl[$;ol]j~T&ap}%ku/2x*>L7F@dP!ʍqۄ̓VH s^Wn {L$_"ZjFnDtѐK '(rPJZn%-JVR \Pxe-pAqܒvyl! 9x<-XyU*SF o;>SS`8 gefx^s#23IDLM" S kt4/SC1ˊ{Nv̋wM&CUW)cu} C&FvR>L#M[gQa4:S|O"sLqp*Kx^{$(&s<ՑkxW(AIq%= .<ǙRʄH|(rWM"2597ޫ|}Ÿڔ2O \-7l6q4ڶ}3y&7%[rBf'cU[2> JనZ by8>yHdQK$'5qC~*og~gqKoۤ>#efuY;zN[wJ Md~, )藪EW+%R[m\fdk>;r4Gmf{2'[` Ѹ2ɛl* БG=۽_n;[&}n~z?{mO]Yl^戴P#1~l>6vz؄&чa]9C~^ֿN}kn5&˼=_=HB4 A*jcDObco $IJvlީv}YM)DBDwt,'ꛟ jXlX&FKcNpݟ_'׉u-2v_'׉{ûE?_;Kz(-wfê$Ĥ"xO";oI ]1l-'oktY4@qS݁WnV^wy1w=K~ݒ/<[v18NL"(S@1/%Nwru5Gg~̎\+%8ߙ&};Nw|o'ۉNo^Ɖvyl'71;d:NmɌVoV3G:Q8ׇLܛou;}Srw   S+  1C(JVi   L Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                     bx[klT>ݵ޵1qQ il6)ID#Յ P4!Vm%R*BZU-%Bgx? zwwy;x~w33g<}?UtL>Qj>*v@R]X hV0BTsbW~GYeПa$Wj6U ')&)XHT۳Rg"BC34"VuЀ=VTlJOSr˟/,PJK͓~UJD,ɃDyH@l`RZIwn)'>1zE`v&ͧ U|}B*C*G*F#F!ݏ4i XqH& g1Ф _mOX dHu :ÑdILo ME&4p֟dI?&7zh~V_V?WFXcZ!T|b3S$~;@oXW?\`/rd ֥ ͉*uEa[0g­ kBnl[$;ol]j~T&ap}%ku/2x*>L7F@dP!ʍqۄ̓VH s^Wn {L$_"ZjFnDtѐK '(rPJZn%-JVR \Pxe-pAqܒvyl! 9x<-XyU*SF o;>SS`8 gefx^s#23IDLM" S kt4/SC1ˊ{Nv̋wM&CUW)cu} C&FvR>L#M[gQa4:S|O"sLqp*Kx^{$(&s<ՑkxW(AIq%= .<ǙRʄH|(rWM"2597ޫ|}Ÿڔ2O \-7l6q4ڶ}3y&7%[rBf'cU[2> JనZ by8>yHdQK$'5qC~*og~gqKoۤ>#efuY;zN[wJ Md~, )藪EW+%R[m\fdk>;r4Gmf{2'[` Ѹ2ɛl* БG=۽_n;[&}n~z?{mO]Yl^戴P#1~l>6vz؄&чa]9C~^ֿN}kn5&˼=_=HB4 A*jcDObco $IJvlީv}YM)DBDwt,'ꛟ jXlX&FKcNpݟ_'׉u-2v_'׉{ûE?_;Kz(-wfê$Ĥ"xO";oI ]1l-'oktY4@qS݁WnV^wy1w=K~ݒ/<[v18NL"(S@1/%Nwru5Gg~̎\+%8ߙ&};Nw|o'ۉNo^Ɖvyl'71;d:NmɌVoV3G:Q8ׇLܛou;}Sr, _:  + F  1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d̢2 0 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    H\ 0 _[W[ ^+APZ(  x  c $@ J   x  c $A OJT      TC k_/k_/ >""%E   x  <xq .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0@d >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0t Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ Bhl =t=   ` @ C 8A K-aceton_pakung+U+*, @ 0| J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0 fCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 00 ,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <T23 |3.58 .& G  @ <: &< |3.58 .& G  @ <x668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ <"2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <|6-0 8 |3.46 .& G  @ <D:;.2J< |3.46 .& G  @ <,F>039@ |3.46 .& G  @ <TQ?RsA i100 K diamagnetic G  @ <[0-4G3 j200 K paramagnetic G  @ <h{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <pr RY S ^aromatic   G  @ <}H@ I ]quinoid G  @ <l~LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13}  @ < Hd  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0h E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0,C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <\P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BjO#)P jCrystals decompose  G  A <^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <` +Y!rZ |3.23 .& G  A <`#Ha&b |3.23 .& G  A < !]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B-s/!2" t3.50 4Gg  A 6`61'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B73*5+ t3.10 4Gg  A Bt=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +rYF T  5F  1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d̢2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    H\ 0 _[W[ ^+APZ(  x  c $@ J   x  c $A OJT      TC k_/k_/ >""%E   x  <xq .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0@d >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0t Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ Bhl =t=   ` @ C 8A K-aceton_pakung+U+*, @ 0| J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0 fCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 00 ,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <T23 |3.58 .& G  @ <: &< |3.58 .& G  @ <x668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ <"2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <|6-0 8 |3.46 .& G  @ <D:;.2J< |3.46 .& G  @ <,F>039@ |3.46 .& G  @ <TQ?RsA i100 K diamagnetic G  @ <[0-4G3 j200 K paramagnetic G  @ <h{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <pr RY S ^aromatic   G  @ <}H@ I ]quinoid G  @ <l~LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13h  @ <o PO  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0h E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0,C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <\P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BjO#)P jCrystals decompose  G  A <^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <` +Y!rZ |3.23 .& G  A <`#Ha&b |3.23 .& G  A < !]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B-s/!2" t3.50 4Gg  A 6`61'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B73*5+ t3.10 4Gg  A Bt=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +r0 {     1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Ori      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|~gin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d̢2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    H\ 0 _[W[ ^+APZ(  x  c $@ J   x  c $A OJT      TC k_/k_/ >""%E   x  <xq .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0@d >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0t Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ Bhl =t=   ` @ C 8A K-aceton_pakung+U+*, @ 0| J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0 fCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 00 ,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <T23 |3.58 .& G  @ <: &< |3.58 .& G  @ <x668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ <"2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <|6-0 8 |3.46 .& G  @ <D:;.2J< |3.46 .& G  @ <,F>039@ |3.46 .& G  @ <TQ?RsA i100 K diamagnetic G  @ <[0-4G3 j200 K paramagnetic G  @ <h{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <pr RY S ^aromatic   G  @ <}H@ I ]quinoid G  @ <l~LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0h E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0,C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <\P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BjO#)P jCrystals decompose  G  A <^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <` +Y!rZ |3.23 .& G  A <`#Ha&b |3.23 .& G  A < !]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B-s/!2" t3.50 4Gg  A 6`61'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B73*5+ t3.10 4Gg  A Bt=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +r R*    1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4dddd̢2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    rކ   )  1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d̢2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    [ 0 ZZ ]+AP'Z(  x  c $@ J   x  c $A OJT    x  <xq .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0@d >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0t Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ Bhl =t=   ` @ C 8A K-aceton_pakung+U+*, @ 0| J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0 fCi @V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  P   E                   G  @ Z wA ,? ?4JS. , @ 00 ,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <T23 |3.58 .& G  @ <: &< |3.58 .& G  @ <x668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ <"2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <|6-0 8 |3.46 .& G  @ <D:;.2J< |3.46 .& G  @ <,F>039@ |3.46 .& G  @ <TQ?RsA i100 K diamagnetic G  @ <[0-4G3 j200 K paramagnetic G  @ <h{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <pr RY S ^aromatic   G  @ <}H@ I ]quinoid G  @ <l~LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0h E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0,C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <\P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BjO#)P jCrystals decompose  G  A <^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <` +Y!rZ |3.23 .& G  A <`#Ha&b |3.23 .& G  A < !]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B-s/!2" t3.50 4Gg  A 6`61'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B73*5+ t3.10 4Gg  A Bt=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +r]   9 L  1C(JVi   Q Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d̢2 0 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    [ 0 ZZ ]+APEZ(  x  c $@ J   x  c $A OJT    x  <xq .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0@d >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0t Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ Bhl =t=   ` @ C 8A K-aceton_pakung+U+*, @ 0| J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0o33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0 fCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4JS. , @ 00 ,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <T23 |3.58 .& G  @ <: &< |3.58 .& G  @ <x668 |3.27 .& G  @ <?bk"]@ |3.27 .& G  @ <"2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <|6-0 8 |3.46 .& G  @ <D:;.2J< |3.46 .& G  @ <,F>039@ |3.46 .& G  @ <TQ?RsA i100 K diamagnetic G  @ <[0-4G3 j200 K paramagnetic G  @ <h{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <pr RY S ^aromatic   G  @ <}H@ I ]quinoid G  @ <l~LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0h E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0,C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <\P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BjO#)P jCrystals decompose  G  A <^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A <` +Y!rZ |3.23 .& G  A <`#Ha&b |3.23 .& G  A < !]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B-s/!2" t3.50 4Gg  A 6`61'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B73*5+ t3.10 4Gg  A Bt=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' 2= @B +r   d i  1C(JVi   V Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 00 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    [ 0 ZZ ]+APEZ(  x  c $AJ  x  c $hBOJT   x  <Xq.  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0b>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0pRa(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B=t=   ` @ C 8A K-aceton_pakung+U+*, @ 0hJ.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0Bn33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0hfCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <X23 |3.58 .& G  @ <: &< |3.58 .& G  @ <L668 |3.27 .& G  @ <h?bk"]@ |3.27 .& G  @ <$2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <`26-0 8 |3.46 .& G  @ <>;.2J< |3.46 .& G  @ <H>039@ |3.46 .& G  @ <XS?RsA i100 K diamagnetic G  @ <]0-4G3 j200 K paramagnetic G  @ <j{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <s RY S ^aromatic   G  @ <thH@ I ]quinoid G  @ <HLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0L  E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0 C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BhjO#)P jCrystals decompose  G  A <<^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A < +Y!rZ |3.23 .& G  A <#Ha&b |3.23 .& G  A <8"!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6X31'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B83*5+ t3.10 4Gg  A B=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +ri x  i  1C(JVi   V Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc,b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0lp4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    [ 0 ZZ ]+APEZ(  x  c $AJ  x  c $hBOJT   x  <Xq.  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0b>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0pRa(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B=t=   ` @ C 8A K-aceton_pakungXU+W, @ 0hJ.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC8 ! ;9IJ @j0Bn33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0hfCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G XB @ 0D 8"'8XB @ 0D 9"'9^B @ 6D >""@A^B @ 6D ):x x Z=^B @ 6D 5  9^B @ 6D 2HH45 @ <X23 |3.58 .& G  @ <: &< |3.58 .& G  @ <L668 |3.27 .& G  @ <h?bk"]@ |3.27 .& G  @ <$2+#.3 |3.46 .& G ^B @ 6D 1**4^B @ 6D 5,,9^B @ 6D 9x.x.,=^B @ 6D >=0=0@A @ <`26-0 8 |3.46 .& G  @ <>;.2J< |3.46 .& G  @ <H      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxy{|}~>039@ |3.46 .& G  @ <XS?RsA i100 K diamagnetic G  @ <]0-4G3 j200 K paramagnetic G  @ <j{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <s RY S ^aromatic   G  @ <thH@ I ]quinoid G  @ <HLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0L  E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0 C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BhjO#)P jCrystals decompose  G  A <<^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A < +Y!rZ |3.23 .& G  A <#Ha&b |3.23 .& G  A <8"!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6X31'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B83*5+ t3.10 4Gg  A B=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +r e   '>  1C(JVi   V Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld-b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    \ 0 [[ ^,AP5[(  x  c $AJ  x  c $hBOJT   x  <Xq.  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0b>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0pRa(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B=t=   ` @ C 8A K-aceton_pakungXU+W, @ 0hJ.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0hfCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G /8 Bj043C ,Aj0B43C@ ! ;9IJ @Bj0n33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ`B @ 0D "8'8`B @ 0D "9'9fB @ 6D ">"@AfB @ 6D x ):x Z=fB @ 6D  5 9fB @ 6D H2H45 @ <X23 |3.58 .& G  @ <: &< |3.58 .& G  @ <L668 |3.27 .& G  @ <hb?k"]@ |3.27 .& G  @ <$+2#.3 |3.46 .& G fB @ 6D *1*4fB @ 6D ,5,9fB @ 6D x.9x.,=fB @ 6D =0>=0@A @ <`2-60 8 |3.46 .& G  @ <>.;2J< |3.46 .& G  @ <H0>39@ |3.46 .& G  @ <XSR?sA i100 K diamagnetic G  @ <]-04G3 j200 K paramagnetic G  @ <j{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <s RY S ^aromatic   G  @ <thH@ I ]quinoid G  @ <HLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1FIf A 0L  E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0 C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BhjO#)P jCrystals decompose  G  A <<^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A < +Y!rZ |3.23 .& G  A <#Ha&b |3.23 .& G  A <8"!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6X31'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B83*5+ t3.10 4Gg  A B=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' = @B +rc> L  ?> `  1C(JVi   V Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld-b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 00p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    \ 0 [[ ^,AP5[(  x  c $AJ  x  c $hBOJT   x  <Xq.  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0b>V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0pRa(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B=t=   ` @ C 8A K-aceton_pakungXU+W, @ 0hJ.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0hfCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4JS. , @ 0,xIY TIn two isostructural salts, KCl4Q" "Me2CO [2] and RbCl4Q" "Me2CO [2], radicals are stacked to form strongly bound dimers (interplanar distances <3.1 , offset <0.9 ). At room temperature, the electron spins of contiguous radicals are paired and the crystals are diamagnetic. About 350 K the crystals decompose and spins decouple, so the samples turn paramagnetic.k.&.&.&.&./&X     G /8 Bj043C ,Aj0B43C@ ! ;9IJ @Bj0n33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ`B @ 0D "8'8`B @ 0D "9'9fB @ 6D ">"@AfB @ 6D x ):x Z=fB @ 6D  5 9fB @ 6D H2H45 @ <X23 |3.58 .& G  @ <: &< |3.58 .& G  @ <L668 |3.27 .& G  @ <hb?k"]@ |3.27 .& G  @ <$+2#.3 |3.46 .& G fB @ 6D *1*4fB @ 6D ,5,9fB @ 6D x.9x.,=fB @ 6D =0>=0@A @ <`2-60 8 |3.46 .& G  @ <>.;2J< |3.46 .& G  @ <H0>39@ |3.46 .& G  @ <XSR?sA i100 K diamagnetic G  @ <]-04G3 j200 K paramagnetic G  @ <j{1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <s RY S ^aromatic   G  @ <thH@ I ]quinoid G  @ <HLM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1Ff A 0L  E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0 C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <7@D9 _heating  G   A <9@D2; _cooling 33 G   A <P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A BgI(,J _heating  G   A BK(,!M _cooling 33 G   A BhjO#)P jCrystals decompose  G  A <<^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A < +Y!rZ |3.23 .& G  A <#Ha&b |3.23 .& G  A <8"!]$^ |3.23 .& G Z 8 '6;- +A'6;-x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A Bs/!2" t3.50 4Gg  A 6X31'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A B83*5+ t3.10 4Gg  A B=]0$2% t3.10 4Gg   A BB-00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??0)H LH  0!M ? 33___PPT10i.;Pw+D=' 6= @B +r   x   1C(JVi   V Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖ"DTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Ld-b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0`p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    r   #  1C(JVi   [ Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc-b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d2 0p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    W 0 WV ],APyV(  x  c $4A J   x  c $B OJT    x  <p .  A series of solvates of alkali salts of tetrachlolrosemiquinone (Cl4Q, chloranil) radical anion were prepared [1] and their crystal structures and magnetic properties were studied. The crystals display a wide range of magnetic properties: they can be paramagnetic, 1D antiferromagnetic or diamagnetic, depending on the distance between ring planes of radicals, which can be modified by different size of alkali cations and solvent molecules. Therefore, their magnetic properties can be tuned by crystal engineering. Electron spins of the contiguous rings are coupled if the interplanar separation is shorter than 3.30 ; they are unpaired if the distance is larger. In acetone solvates, KCl4Q" "Me2CO and RbCl4Q" "Me2CO, strongly bound radical dimers in the singlet state exist; therefore the crystals are diamagnetic [2]. In acetonitrile solvate, NH4Cl4Q" "MeCN, infinite stacks of equidistant anions (interplanar separation 2.227 ) occur; therefore the crystals are 1D antiferromagnets. The most interesting example is ethylmethylketone solvate KCl4Q" "EtCOMe which displays a continuous, reversible, single crystal-to-single crystal phase transition in the range 120 - 170 K. In the low-temperature phase (100 K), strongly bound dimers with paired electrons occur, similar to those in KCl4Q" "Me2CO. However, in the high-temperatre phase (200 K), infinite stacks of equidistant radicals are detected; electron spins are unpaired due to greater interplanar distance. Spin coupling was also confirmed by ab initio quantum chemical calculations. Cn  !(        > ?       E    @   :  "     U   q   /  & r8X  0 H >V3SIb  Nucleus Independent Chemical Shift (NICS) values calculated along the axes perpendicular to the quinone ring for the neutral quinone, radical anion - semiquinone, hydroquinone dianion and the benzene are shown. The NICS profiles for neutral quinone species are typical for nonaromatic molecules, while those for hydroquinone dianions are typical for aromatic species, although notably less aromatic than the prototype benzene. [2] p-Tetrachlorosemiquinone aromaticity is in between the bordering cases, benzene and quinone.X (2\$ 7                )  ^ ` G  " 0 Ra(IMh R|Conclusions -Interactions of semiquinone radical anions observed and described for the first time. Multi-atom centered bonding occurring in radical dimers with -systems offers unique characteristics. The reversibility and dynamic nature of this bonding provide the possibility to design swichable molecular systems.\ 2 ('1&H G  \ B =t=   ` @ C 8A K-aceton_pakungXU+W, @ 0, J.J0 KCl4Q" "MeCOEt: Structural changes induced by increased temperature are accompanied by changes of magnetic propertiesu(((.(((f( uG l @ C DA,KCl4Q-EtOMe-pak_ortepj0EC !  `q A ? ?0e3LJ}B r @ S JA ,800px-Loligo_vulgarisv27c?8 @ 0T fCi ^V[1] H. A. Torrey, W. H. Hunter, J. Am. Chem. Soc., 1912, 34, 702-716. [2] K. Mol anov, B. Koji-Prodi, D, Babi, D. }ili, B. Rakvin, CrystEngComm. 2011, 13, 5170-5178.  L   E                   G  @ Z wA ,? ?4J:- ,/8 Bj043C ,Aj0B43C@ ! ;9IJ @Bj0n33Cj @ C :A"stekovi-EMK-100K! ;X-IJZ @ C *A EMK_200K:- ;9IJ`B @ 0D "8'8`B @ 0D "9'9fB @ 6D ">"@AfB @ 6D x ):x Z=fB @ 6D  5 9fB @ 6D H2H45 @ <H 23 |3.58 .& G  @ < : &< |3.58 .& G  @ < 668 |3.27 .& G  @ < b?k"]@ |3.27 .& G  @ <$ +2#.3 |3.46 .& G fB @ 6D *1*4fB @ 6D ,5,9fB @ 6D x.9x.,=fB @ 6D =0>=0@A @ </ -60 8 |3.46 .& G  @ <; .;2J< |3.46 .& G  @ <> 0>39@ |3.46 .& G  @ <Q R?sA i100 K diamagnetic G  @ <H\ -04G3 j200 K paramagnetic G  @ <h {1k9<2 ]SQUID G 8 DV A,D029IUR @ C "A NICSDVZB @ s *Do,xUjUZB @ s *Do+_EihEZB @B s *Do YE,xUZB @B s *DoleExUL @ C BCCDEdF,A3 &&Ld {^Vwx  ^ 1  .eN7(C!@        "`,JoN`B @B 0D3 H\H @ <|r  RY S ^aromatic   G  @ < } H@ I ]quinoid G  @ <T LM FN  Cl4Q" -Lfff.f G P @ C (Arudjer13'  @ <Ĕ o >O  F300th anniversary of Ruer Boakovi$$ $G f @ c >xANH4Cl4Q_pak1Ff A 0,  E<= hKCl4Q" "Me2CO and RbCl4Q" "Me2CO: diamagnetic crystals5(((.((( ((((((( 5G b A 0ċ C6_uE BNH4Cl4Q" "MeCN: 1D antiferromagnet"(((((.(( "G  A <D 7@D9 _heating  G   A < 9@D2; _cooling 33 G   A <p P=>8I> nReversible transition!  G L Q4KQI1Z A# 6F0V @ Z A B? ?Q4KQI1Z B @ Z ~A C? ?A8KQCS C A Bh gI(,J _heating  G   A B K(,!M _cooling 33 G   A B jO#)P jCrystals decompose  G  A <H ^x _ kEquidistant anions:  G 8 V')e AW)uf| @ s LA"amonij_MeCN-stekV')elB @ <DԔ"`"clB A <DԔ \ `lB A <DԔJXJ[ A < +Y!rZ |3.23 .& G  A < #Ha&b |3.23 .& G  A <4" !]$^ |3.23 .& G Z 8 '6;- +AUD(q6v+x A HAKCl4Q-stack'6;-lB A <DԔ 1' 1#)lB A <DԔ.[!.g# A B s/!2" t3.50 4Gg  A 6H2 1'4( t3.50 4Gg lB A <DԔ2)*2+lB A <DԔ/m$/&lB A <DԔ,,T  A BD7 3*5+ t3.10 4Gg  A B= ]0$2% t3.10 4Gg   A BB -00 t3.10 4Gg fB !A 6D ]0%]0&fB "A 6D -- fB #A 6D 3+3,fB $A 6D 3)3*fB %A 6D ]0#]0$fB &A 6D --x )A c PA ,800px-Loligo_vulgarisFx 'Lx @ <A L??,)H  LH  0!M ? 33___PPT10i.;Pw+D='  = @B +rT# 1  0#  1W(JVi   ` Graph Origin50.Graph0Origin GraphL  ISIS/Draw Sketch ISISServer0 ISIS/Draw Sketch,  Graph Origin50.Graph0Origin GraphB  Graph Origin50.Graph0Origin GraphC  Graph Origin50.Graph0Origin Graph/ 0DArialn Old StylPPsؖ2 0ؖDTimes New RomanPPsؖ2 0ؖ DBookman Old StylePsؖ2 0ؖ B.G  @n?" dd@  @@`` Lc-b$|߃/'A!2$C4 7-HA(R$}ETY-biPq2$X?`T9QR$1|GCٮNiiab$LxP4̛_Q1sb$+Ѳ? ]+b$|>b!&sd$!ByYqb$bfIzU)jSR$'}IVw h74d$2$0{r}G^C_`!2$ --.Zys5yv"2$<(_MUlb"b${s >l*o"b$zjš!pI4o=lK$ 0AA`3f33@wʚ;ʚ;g4!d!d$2 0 p4pA%<4dddd 0Pr <4BdBd8 0P80___PPT10 pp?  %-INTERACTIONS OF SEMIQUINONE RADICALS: CRYSTAL DESIGN AND TUNING OF THE MAGNETIC PROPERTIES >^'H[HH0[  Kreaimir Mol anov and Biserka Koji-Prodi Rudjer Boakovi Institute, Bijeni ka c. 54, Zagreb, Croatia; E-mail: kmolcano@irb.hrF00=00                    rщ   0  1