ࡱ>  !@ Qbjbj.. v\DD| $ Pl0< Bzxx({{{T0V0V0V0@0D8DA$sDRF BAq |{{||BA B|% T0|T0| tl B.!PB0BbGp6G$t G tL{r\{{{BABA صD  صLuminescence and Raman spectra of acetylacetone at low temperatures Vlasta Moha ek-Groaeva,* , Kreaimir Furia and Hrvoje Ivankovib aRuer Boakovi Institute, POB 180, Bijeni ka c. 54, 10002 Zagreb, Croatia, b Faculty of Chemical Engineering and Technology, Maruliev trg 19, 10000 Zagreb, Croatia e-mail: mohacek@irb.hr . TITLE RUNNING HEAD Luminescence in acetylacetone ABSTRACT Raman spectra of acetylacetone were recorded for molecules isolated in an argon matrix at 10 K and for polycrystalline sample. In solid sample broad bands appear superimposed on much weaker Raman spectrum corresponding to the stable Cs enol. Their position depends on the excitation wavelength (514.5 nm and 488.8 argon ion laser lines were used), sample temperature and cooling history. These bands are attributed to transitions from excited higher electronic state to various isomer states in the ground electronic state. Laser photons excite acetylacetone in crystal in the region where a number of excited triplet states are predicted for a free acetylacetone molecule (X.B. Chen et al. J. Phys. Chem. A 110 (2006) 4434.). Since singlet to triplet photon absorption transitions are forbidden, states existing in solid have mixed singlet/triplet character. Their decay results in population of different isomer states which are not vibrationally resolved except for the lowest isomers: Cs enol, C2v enol (here denoting possibly both TS1 and TS2 transition states described in Matanovi and Doali, J. Phys. Chem. A 109 (2005) 4185.), and keto form which can be detected in solid Raman spectra. Differential scanning calorimetry showed two signals on cooling of acetylacetone, one at 229 K and one at 217 K, while on heating they appear at 254 K and 225 K. The phase change at higher temperature is attributed to freezing/melting transition, while the one at lower temperature seems to correspond to freezing/melting of keto domains as suggested by Johnson et al. [ J. Chem. Phys. 116 (2002) 5694]. Using matrix isolation in argon technique, vibrational spectrum of acetylacetone at 10 K was recorded. Two bands at 3113 cm-1 and 3083 cm-1 are assigned to methyne CH stretching vibration of Cs and C2v enol conformers. Strong bands at 1602 cm-1 and 1629 cm-1 are assigned as Cs enol bands, and weaker underlying band at 1687 cm-1 and medium band at 1617 cm-1 as C2v enol bands. KEYWORDS: Fluorescence, singlet-triplet mixing, methyl group, enol-keto tautomerism, isomers INTRODUCTION Acetylacetone (2,4-pentanedione), acac, serves as a model for the study of intramolecular hydrogen bonding, together with other  diketone molecules1. It is often used as a complexing agent with various metal ions2,3, and in producing compounds for organic light emitting diodes4. It is a rather small molecule, but of rich dynamics exhibiting effects of tautomerism. In the simplest model two molecular species, enol and keto, are existing in equilibrium at room temperature in the approximate ratio 3:1 in the favour of enol1 (see Fig 1.). Temperature5 and solvents6 are known to affect this ratio and move it either towards enol or keto side. The potential energy surface that determines the positions of tautomer minima has been intensively studied7-18. Matanovi and Doali performed quantum calculations of vibrational states and stable conformers of acetylacetone10. They found two transtion states in the vicinity of the global minimum (which is a Cs enol): the TS2 transition state, that is 0.26 kcal/mol higher in energy han the ground state and corresponds to enol tautomer with symmetrical methyl groups and asymmetrically placed hydroxyl hydrogen, and the TS1 proton tranfer transition state which is 2.64 kcal/mol higher than the ground state in which hydroxyl proton is midway between oxygens and methyl groups are as in TS2, calculated at the MP2(FC)6-311+G(d,p) level of theory10. Both in TS1 and in TS2 methyl groups are identically oriented and major differences in conformation concern the hydroxyl proton and the electron density distribution in the ring. These slight variations are often impossible to detect in the experimental data, and in the literature one often finds reports on the existence of the second acac enol conformer - C2v enol. After the discovery of Veierov et al.19 that acetylacetone displays isomerization upon UV illumination, number of studies were devoted to isolation of different isomers and calculation of their relative energies20-27. Special attention was given to methyl groups, since their inequivalence, if found, would support an unsymmetric planar Cs structure as oposed to symmetrically planar C2v. Two different methyl tunneling transitions were observed for pure enol crystalline sample and different barrier heights assigned to two methyl groups using neutron diffraction28-32. 13C NMR spectra of acetylacetone embedded in host matrix33 or 1H NMR spectra of acac in various solvents6 and deuteron NMR spectra were collected34. High resolution rotational spectra supported C2v equilibrium structure35, just as electron diffraction experiments of Lowrey et al.36, but contrary to electron diffraction experiments of Iijima et al.37 and Srinivasan et al.38 who argued that planar but non-symmetrical Cs structure was the most stable. In pure solid acetylacetone a disorder of hydroxyl protons in molecules occupying C2v sites in the crystal was observed by X ray diffraction39 while planar non-symmetric enol Cs structure was identified as residual solvent in crystals of antiepileptic drugs40. Vibrational studies of acetylacetone gave a thorough assignment of bands41-45 for enolic Cs tautomer, and some, more intense bands of keto tautomer that could be observed, since approximately 25 % of molecules are in keto form at room temperature6. Chiavassa et al. first performed infrared matrix isolation experiments42 and later Coussan et al. included induced UV and IR isomerizations22. No Raman spectra of matrix isolated acetylacetone are reported in literature, and tabulated wavenumbers of observed bands in solid were given by Tayyari41. We undertook the Raman matrix isolation experiment to verify the conclusion of Cohen and Weiss5 and Tayyari41 that there exist two enolic forms rapidly interconverting in the liquid. Also, low temperature Raman spectra of polycrystalline sample were collected from 10 K to 300 K for the study of possible disorder of methyl groups. EXPERIMENTAL METHODS Acetylacetone (acac), 99.5 % pure, was purchased from Sigma-Aldrich (Fluka) and transferred to a capillary tube with several freeze-pump-thaw cycles performed to eliminate dissolved air. The capillary was sealed under vacuum. For low temperature measurements we used several cryostats: an old CTI model 21 CRYOGENICS, a new CCS350 JANIS RESEARCH, both with closed cycle of liquid helium which could reach 10 K, and a VPF 700 from JANIS RESEARCH operating with liquid nitrogen for temperatures as low as 80 K. For temperature control Lake Shore 331 instrument was used. For matrix isolation experiment, a small amount of pure liquid acac was transferred into glass vial and freeze-pump-thaw cycles repeated. The vial with frozen sample was evacuated with rotatory and diffusion pumps, and then connected to a Swagelok needle valve leeding to the cold golden plated cryostat finger on one side, and to the reservoir of argon on the other. The vapour pressure of liquid acac is 0.8 kPa (from Sigma-Aldrich web site). After the sample melted at room temperature, acac vapour was allowed to mix with argon from the reservoir held at pressure of 1 atm. by opening the valve towards argon. The matrix ratio was estimated from the ratio of pressures of acetylacetone vapor and argon and was approximately 1:100. The vapor/gas mixture was deposited on the golden surface inside the cryostat head cooled to 10 K. The traces of air were found (2328 cm-1 from N2 stretching band and 1554 cm-1 from O2 stretching band), because of imperfect sealing. Differential scanning calorimetry experiment was performed with Netzsch DSC 200 instrument equipped with liquid nitrogen cooling system in He atmosphere. The cooling rate was 5 K/min, and heating rate was also 5 K/min. Raman spectra were recorded with DILOR Z24 Raman spectrometer, while excitation was provided with argon ion laser COHERENT INNOVA 400 operating at 514.5 nm and 488.8 nm with laser power of 200 mW at the sample. Spectra were recorded in sequential mode, step size used ranged from 0.5 cm-1 to 4 cm-1. Slitwidth was 300 m. RESULTS Matrix isolation experiment Infrared and Raman spectra of liquid acac are shown in Fig 2., and Raman spectrum of matrix isolated sample in Fig. 3. The positions of observed bands are listed in Table 1. All 39 normal modes of Cs enol are active in Raman and infrared, and for C2v enol, modes symmetry is ( = 13 A1 ( 6 A2 ( 8 B1 ( 12 B2. All modes are Raman active, but A2 modes are infrared inactive. Among the A2 modes there is one CH stretching from methyl groups, one HCC bending mode of methyl groups, an out of phase in plane methyl group bending, an out of phase out of plane bending of methyl groups, a ring torsion and a methyl torsion mode. Coussan22, Nagashima23, and Chiavassa42 recorded infrared spectra of matrix isolated acac. Nagashimas values for argon matrix agree rather well with our reported values (Table1), and we could provide bands below 500 cm-1, neither of which were reported previously. Generally, there are no bands corresponding to keto isomer in the spectrum of matrix isolated acac, but there is a superposition of weaker and broader bands onto stronger and narrower bands falling at the same wavenumber: such is the case of a weak band at 1687 cm-1 underlying the stronger one at 1629 cm-1. The band at 1687 cm-1 we assign to quasiaromatic carbonyl stretching band in the symmetric C2v enol, and the band at 1629 cm-1 to the Cs enol. The shoulder at 1617 cm-1 is assigned as the C2v enol band, and the strong band at 1602 cm-1 as belonging to the Cs enol. Another characteristic band of C2v enol we found at 3082 cm-1 which corresponds to CH stretching vibration of the methyne hydrogen, while CH stretching of the Cs enol methyne group is found at higher wavenumber (3113 cm-1). Two other bands involving methyne group that are sensitive to the enol state are according to ref [7] in plane CH deformation predicted to be at 1183 cm-1 for Cs enol, and at 1178 cm-1 for C2v enol, and out of plane CH deformation predicted to lie at 766 cm-1 for Cs isomer, and at 758 for C2v enol. We observed a shoulder at 1184 cm-1, a medium band at 1175 cm-1, and weak bands at 786 cm-1 and 774 cm-1. Upon careful inspection of the spectrum for hydrogen bond transitions, we could not confidently assign any. The weak band at ~ 3500 cm-1 was also observed in another matrix isolation experiment we performed after this one, but no band of acetylacetone was simultaneously observed. Therefore the 3500 cm-1 band is most probably caused by remains of methanol that was used for cleaning of the apparatus. Nagashima et al.23 also observed weak band at 3500 cm-1 in infrared matrix isolation experiments and assigned it to small amounts of water interacting with acetylacetone. The bands at 2855 cm-1 and 2721 cm-1 are observed in liquid and in polycrystalline solid as well, and can be assigned as combinations: (1602 + 1250 cm-1) and (1296 + 1435 cm-1). A weak band at 365 cm-1 is a ring bending mode involving oxygen atoms41. Raman spectra of polycrystalline acetylacetone On cooling, liquid acac freezes at 229 K and has a solid-solid phase transition at 217 K (Fig. 4.), whereas on heating these phase changes occur at higher temperatures - at 254 K and 225 K. The transition at higher temperature is the freezing/melting transition, while the lower one probably involves the freezing/melting of the keto domains as suggested by Johnson et al.28. Rapid cooling of liquid invariably produced a mixture of enol and keto crystalline domains (Fig. 5, top and middle Raman spectra). The procedure applied by Johnson was to perform annealing at 245 K for ten hours. The sample thus produced was pure enol polycrystalline powder28, whose crystal structure corresponded well with the one determined by Boese et al.39: space group Pnma with four molecules per unit cell and molecular site symmetry C2v. The activity of optical phonons is (opt ph = 3Ag ( 3B1g ( 3 B2g ( 3 B3g ( 3 Au ( 2B1u ( 2 B2u ( 2 B3u. All twelve gerade phonons are Raman active, and six phonons of B1u, B2u, and B3u symmetry are infrared active. Eight low frequency bands in Raman spectrum of polycrystalline enol acac were assigned as lattice vibrations (Fig. 5a). After annealing, only enol bands were observed (Fig. 5 bottom spectra). Very broad bands of medium and strong intensity accompanied all Raman spectra and are discussed in the next section. There is different intensity distribution among the internal modes, depending on the cooling procedure and the amount of enol conformer produced. It is often possible to observe the situation where at 10 K the band at 1296 cm-1 is stronger than the band at 1605 cm-1 (Fig 5. spectrum at the top), while in another cooling, again at 10 K, the ratio is reversed (Fig. 5, middle spectrum). In Table 1 all observed bands are listed, as well as those of keto conformers such as the bands at 1711 cm-1, 1700 cm-1, 975 cm-1, 624 cm-1, and 534 cm-1 . Phonon spectra of the annealed sample (spectrum at the bottom of Fig. 5.) and of the sample that was rapidly cooled (at the top and in the middle of Fig. 5) differ in the ratio of intensities of the 63 cm-1 and 101 cm-1 phonon band, and in the appearance of the weak phonon at 27 cm-1 which is assigned as the keto lattice phonon. Methyl group vibrations fall in four distinct frequency intervals: stretching vibrations, bending vibrations of the HCC angles, bending of HCH angles and methyl torsions. The vibrations at 1000 cm-1 and 1025 cm-1 are most probably HCH deformation bands of the Cs enol, whereas the band 1040 cm-1 could correspond to such vibration in one of symmetrically positioned methyl group. Tayyari41 gave a thorough assignment of Cs enol vibrations, giving values of vibrations in solid at undefined higher temperature (higher than 80 K since he did not observe the splitting of 1634 cm-1 and 1652 cm-1 bands , but reported one band instead). Luminsescence in polycrystaline acetylacetone Luminescence bands are reported to appear together with Raman spectra of organic solutions46, in supraconductors47 and conjugated polymers48. Usually vibrational spectroscopists attribute the term luminescence to bands which appear in Raman spectra at different wavenumbers when different laser lines are used for excitation (their Raman shift varies), but are at the same absolute wavenumbers. In Figures 6 and 7 temperature dependent Raman spectra of acac are shown. They were obtained when green (Fig 6.) or blue (Fig 7.) laser line served as the excitation source. Strictly speaking, the observed broad bands are not luminescence bands in the sense just mentioned, because there are more of them when blue line is used and their position somewhat changes. Still, we shall keep the term for the lack of better one, since in our experiments we cannot distinguish between fluorescence (light emitted from higher to lower vibrational states in the excited electronic state) and phosphorescence (light emitted when molecules relax from the lowest vibrational state in the excited electronic state into vibrational states of the ground electronic state). DISCUSSION Among systems displaying keto-enol tautomerism such as 1-hydroxyanthraquinone49 or 2-(2'-hydroxyphenyl)benzoxazole50, enol and keto singlet and triplet states are close in energy and upon excitation a number of relaxation pathways opens. Similar situation is found in acetylacetone, whose excited electronic states were studied by Chen et al.8, Nakanishi et al.20, Coussan et al.21, Nagashima et al.22, and Upadhyaya et al.25 among others. Strong UV band appearing at 266 nm in the absorption spectra corresponds to S0 ( S2 transition, the S2 state decays into lower S1, T2 and T1 states, which decay further into ground states of different acac isomers20-27. Notation used to describe the isomers consists of three capital letters CCC, CTC etc. The first letter refers to conformation with respect to rotation around carbon-carbon single bond in the ring, the second letter describes conformation with respect to rotation around the double carbon bond, and the third letter refers to conformation with respect to rotation around the carbon-hydroxyl oxygen bond. Absorption selection rules for photons forbid singlet to triplet transitions, but it is known that in the solid the excited states are not pure singlet or triplet states48. In Fig. 8. energy level diagram showing data from Matanovi and Doali10, Nagashima et al.22, and Chen et al.8 is presented. Not all transition triplet states listed in [8] are shown, because of clarity. One can see that in the region of our green laser excitation (19436 cm -1) the enol triplet state of free acac molecule E(T1) is predicted at 19845 cm-1 8, while around the energy of the blue argon ion laser line (20458 cm-1) three states are predicted at 20405 cm-1, (CTT(T1)), 20440 cm-1 (CCT(T1)) and 20545 cm-1 (TCC(T1))8. Because electronic states in solid have bandwidths of the order 1600 cm-1 51, these states are accessible with our laser excitation. In Table 2. we give the tentative assignment of the broad bands observed in polycrystalline acac shown in Figs. 6 and 7. While in matrix isolation experiments no luminescence bands were observed because molecules interacted less with one another, in polycrystalline solid the intermolecular interaction causes the changes in the nature of excited electronic states of acac from pure triplet to mixtures of singlet and triplet states. CONCLUSION Light scattering experiments on acetylacetone at low temperatures display a number of strong broad bands appearing beneath Raman spectra of solid. These results are interpreted as transitions from molecules excited to higher states to various isomers in the ground electronic state. Laser photons of energies 19436 cm-1 and 20458 cm-1 excite acac in the region where a number of excited triplet states are predicted for free acetylacetone molecule. Since singlet to triplet photon absorption transitions are forbidden, we conclude that states existing in solid acac have mixed singlet/triplet character. Their decay results in population of different isomer states which are not vibrationally resolved except for the lowest isomers: TS1 and TS2 transition states (jointly denoted C2v enol) and keto form which can be detected in solid Raman spectra. Molecular conformation of matrix isolated acetylacetone is dominantly Cs enol, but the bands corresponding to enol conformers with symmetrically placed methyl groups (C2v enol) are also observed. ACKNOWLEDGMENT This work was made possible by the grants 0098019, 0098022 and 0125019 of Ministry of Science, Technology and Sport of the Republic of Croatia. Figure captions Figure 1. Different tautomers, enol and keto, of acetylacetone. Figure 2. Infrared and Raman spectra of liquid acetylacetone. Figure 3. Raman spectrum of acetylacetone isolated in argon matrix at 10 K. Matrix ratio ~ 1:100. Figure 4. Differential scanning calorimetry signal of acetylacetone. Heating rate 5 K/min, cooling rate 5 K/min. Figure 5. Low temperature Raman spectra of polycrystalline acetylacetone at 10 K. a) interval 2600 - 3300 cm-1, b) 100 - 1800 cm-1 interval, c) phonon spectra 10 - 130 cm-1. Excitation wavelength 514.5 nm, laser power 200 mW, slitwidth 300 m. Figure 6. Temperature dependent Raman spectra of acetylacetone displaying strong broad luminescence bands corresponding to frozen relaxation from higher energy isomers (see text). Excitation wavelength 514.5 nm (19436 cm-1) . Figure 7. Temperature dependent Raman spectra of acetylacetone displaying strong broad luminescence bands corresponding to frozen relaxation from higher energy isomers (see text). Excitation wavelength 488.8 nm (20458 cm-1). Figure 8. Energy level diagram of acetylacetone ground and excited states based on predicted values for TS1 and TS210 , E(T1), TCC(T1), CCT(T1) and CTT(T1)8 and the rest from ref [23]. Not all states are shown, please see references mentioned for the fuller list. Table 1. Observed Raman and infrared bands of acetylacetone (cm-1). Raman matrix 10 K Raman solid 10 K enols+keto Raman solid 10 K enols+keto Raman solid 10 K enols Raman liquid 295 K enols+keto Infrared liquid 295 K enols+keto Assignment 4906 m,vbr4900 vs,vbr5354 vs,vbr3496 vwimpurity, CH3OH? 3113 w3109 mw3114 w3113 mwCH stretching Cs enol3095 w,br 3093 mw,sh 3089 mw3086 w3075 w,sh3082 w3081 wCH stretching C2v enol3014 mw3016 m3017 m3008 mw CH3 asym stretch.3009 mw3004 mw,sh3009 m3003 mCH3 asym.stretch.  2979 m2981 mw,sh2980 w,sh CH3 asym. stretch.2973 mw,sh2969 s2968 m2969 s2965 m,sh 2968 mwCH3 asym. stretch.2934 vs2925 vs2924 vs2925 vs2925 vs 2928 mwCH3 sym.stretch.2855 w,br2841 w2847 vw2849 w,br2846 w 2844 wcombin.or hydr. bond transition ? 2796 w2721 w2719 vw2714 w 2707 wcombination 2636 w2328 s N2 stretch1994 wcombination1800 m,vbr1922 wcombination Table 1. continued Raman matrix 10 K enols Raman solid 10 K enols+keto Raman solid 10 K enols+ keto Raman solid 10 K enols Raman liquid 295 K enols+keto Infrared liquid 295 K enols + keto Assignment 1715 w1715 vvw1732 w1730 sC=O stretch keto 1700 w1698 vvw1709 sC=O stretc keto1687 w,sh1683 w1672 br,shCO str.C2v enol1651 mw.sh1653 mw,sh1652 mw,shC=O str. Cs enol1629 m,sh1634 m1638 mw1634 ms1622 vs,vbrC=C-C=O str Cs enol1617 m,shC=C-C=O str C2v enol1602 s1605 m1605 m1607 ms1604 s,brC=O + (O-H) Cs enol1585 mw,sh1583 mw1585 m1554 mO21495 vw1490 w,sh1464 w1455 m1454 m1455 m1462 m,shCH3 asym. bend.1445 mw,sh1441 mw1442 mwCH3 asym. bend.1434 mw1433 mw,brCH3 asym. bend.1423 w,sh1425 mw1427 m1426 m1424 s,brCH3 asym. bend.1406 w1408 w,sh1409 w1375 m1378 ms1377 m1378 s1372 ms1363 sCH3 sym. bend.1367 m,sh1355 w,sh1354 w1355 wCH3 sym. bend.1309 mw,sh1310 w,sh1308 mw,sh1300 s,vbr1296 s1296 m,br1297mw,br1298 ms1296 s,br1307 msO-C=C-O,(O-H) Cs enol Table 1. continued Raman matrix 10 K enols Raman solid 10 K enols+keto Raman solid 10 K enols+ keto Raman solid 10 K enols Raman liquid 295 K enols+keto Infrared liquid 295 K enols + keto Assignment 1250 s1247 m1249 mw,br1248 m1252 s1250 sC=C-C sym.str Cs enol1235 ms,sh1240 mw,shC--C--C stretch. C2v enol1184 w,sh (CH) in plane, C2v enol1175 m1173 mw1174 m1173 m1176 mw1172 m (CH) in plane, Cs enol1100 w,vbr1104 w,br1157 m1040 mw1039 w1039 w1039 w 1036 w1052 w,shCH3 def. out of pl.1016 mw,sh1025 mw1026 w1026 mw1024 mCH3 def out of pl.1005 mw,sh  999 m1001 m1001 ms 1000 s 999 m1003 mCH3 def. in plane 975 vw 957 mketo band 934 w 941 m941 s940 ms931 mw(C=C-C) bend. 919 w,sh 919 w921 mw917 w 915 msC-CH3 stretch Cs enol 910 w 910 w,sh910 mw,sh908 mw,sh 913 w,shC-CH3 stretch C2v enol 902 mw904 mw899 m817 mw817 w786 w,sh807 w806 w,sh (CH) out of pl.C2v enol 797 mw 797 m798 m Table 1. continued Raman matrix 10 K enols Raman solid 10 K enols+keto Raman solid 10 K enols+ keto Raman solid 10 K enols Raman liquid 295 K enols+keto Infrared liquid 295 K enols + keto Assignment  774 w788 w787 w787 mw 789 w,as782 m,as(CH) out of pl.Cs enol 770mw,br725 w,sh 647 s 648 s 648 ms649 s 643 mwin plane ring bend. Cs enol 635 s 642 s642 ms643 s 645 sout of pl. ring def. Cs enol  624 mw 623 ms,sh621 mw,shketo band 615 w,sh 583 w 555 mw 555 ms 554 m554 ms 556 mout of pl. ring def. Cs enol 534 vw  530 vw 531 mwketo band 509 w 504 m 505 mw504 m 510 vw513 mwin plane ring bend.Cs enol 450 w,vbr453 w,br  413 w 413 w412 win plane ring def.Cs enol 406 vw 404 w 406 vw403 w 406 win plane ring def.C2v enol 365 vw 358 w,br 353 w355 w,br 372 wring bending 340 w,sh   330 wKeto band  235 mw 234 mw236 mw 225 w226 mw,sh 228 mwring bending203 mw,sh 192 w 198 m196 ms197 mring def. +CH3 torsion 174 w170 mw174 w 158 w 155 w153 w155 w 160 m,shring def. +CH3 torsion 113 mw,sh 101 s 101 vs105 slattice vibration 86 m,br 89 ms 90 mwlattice vibration 71 m  73 ms 74 mlattice vibration Table 1. continued Raman matrix 10 K enols Raman solid 10 K enols+keto Raman solid 10 K enols+ keto Raman solid 10 K enols Raman liquid 295 K enols+keto Infrared liquid 295 K enols + keto Assignment  62 vvs 63 vvs 65 vvslattice vibration +CH3 torsion  55 ms 55 wlattice vibration 48 w,sh 47 m 48 wlattice vibration 39 w 41 wlattice vibration 34 w 35 m 35 wlattice vibration 27 wketo lattice phonon Abbreviations: v -very, s - strong, m - medium, w - weak, as - asymmetric, sh shoulder, br - broad Table 2. Observed broad bands underlying low temperature Raman spectra of Cs enolic acetylacetone. "C2v enol" refers to unresolved superposition of TS1 and TS2 transition states10. Excitation 0 = 514.5 nm 0 = 19436 cm-1Excitation 0 = 488.8 nm 0 = 20458 cm-1T(K)R (cm-1)0 - R (cm-1)AcAc isomer giving origin to the bandT(K)R (cm-1)0 - R (cm-1)AcAc isomer giving origin to the band 230 200 180 150 90 40 10 4500 700 4250 720 4200 2900 2600 950 5000 4525 950 4750 1110 4800 1025 4850 101014936 18736 15186 18716 15236 16536 16836 18486 14436 14911 18486 14686 18326 14636 18411 14586 18426 CTT C2v enol + keto CTT C2v enol+ keto CTT C2v enol + keto TCC CTT C2v enol + keto CTT,TCC C2v enol+ keto CTT,TCC C2v enol + keto CTT,TCC C2v enol + keto 235 215 150 100 80 50 10 4000 1500 4000 1490 6040 4010 1430 5760 4030 1400 5820 4050 1530 5820 4040 1490 5818 4045 154016458 18958 16458 18968 14418 16448 19028 14698 16428 19058 14638 16408 18928 14638 16418 18968 14640 16413 18918 CTC C2v enol + keto CTC C2v enol + keto CCT CTC C2v enol + keto CCT CTC C2v enol + keto CCT CTC C2v enol + keto CCT CTC C2v enol + keto CCT CTC C2v enol + keto REFERENCES: 1. Emsley, J. Structure and Bonding, 57 (1984) 147. 2. Imao, T; Noma, N; Ito, S J. Sol-Gel Sci Techn. 38 (2006) 197. 3. Saryuk, V. T.; Zolin, V.; Legendziewicz, J.; Szostak, R.; Sokolnicki, J. Spectrochim. Acta A61 (2005) 185. 4. Zhang, R.-J.; Yang, K.-Z.; Yu, A.-C.; Zhao, X.-S. Thin Solid Films 363   V X     q r s x y ) * ƿͬ|xh% hvH*\ hv\hQf hs5hshQf5 h5 hv1hv1 hshF hQfhF hF5 hFh hshv hFhFhFhs hv6]hvhv]hvhvH* hvhv hvH*h*hv- X  `gd3*gd3gd%gdv1$gdgd3$gdFgdF$gd3gd3gd3gd3QQ* f l (;KLO^xefghnoqvw,FLNT  !"#TVqswxzĽĸijijĩĩijijĩijijĩh%hv5H*\h%hv5\ hvH* hv\ hv6]hv h(6 h 6hM}h 5 h 5H* h 5hM h%5 h%6h%h1Kh >:<>@~LXdBDE|~:@G H I v ûӷӷðӫ÷ûû h1KH* h;5\hFh5H*\ h5\h33@ h33@H*hhhQf5 hQfh;h*h1K hQfhQf hQfh*h%C#)&~''')-x.y. 0 00T04c9<<<<<cAC HHH=HLgd3v w y *!/!1!3!5!i!k!o!p!!!!!!!! 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lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd6~$$Ifl   ֞ 8/(    n  j  t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd|$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd>$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdŽ$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdF$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdʙ$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdN$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdҤ$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdV$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdگ$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(    n  j  t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdf$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd($$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdn$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd0$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kdv$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd8$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd~$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd@$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j #v#v#v#v#vn#v#vj :V-l t)55555n55j kd$$Ifl   ֞ 8/(nj t0  )44 lapF$$If!vh55555n55j 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