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RP\!V$EI]|6']HukÐ8Fca{/Q؀Ó]hu)~ H.J^.9~/֩NKBEfF$4.kL;QMmQ7:F^c}x+t(C5ՎLAM3Vl_->),QCn:Jq ,8fjЮU *.'11B~z1X&YklAeh9y2%-C> endobj 671 0 obj <> endobj 672 0 obj <> endobj 673 0 obj <> endobj 674 0 obj <> endobj 1 0 obj <> endobj 2 0 obj [3 0 R 4 0 R 5 0 R 6 0 R 7 0 R 8 0 R 9 0 R 10 0 R 11 0 R 12 0 R 13 0 R 14 0 R 15 0 R 16 0 R 17 0 R 18 0 R 19 0 R 20 0 R 21 0 R 22 0 R 23 0 R 24 0 R 25 0 R 26 0 R 27 0 R 28 0 R 29 0 R 30 0 R 31 0 R 32 0 R 33 0 R] endobj 3 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compounds.\ a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the intrinsi\ c Mott physics is the Mott Hubbard ba:2517)/F 4/H/N/Rect[80.9548 108.32 113.532 94.2767]/Subtype/Link/Type/Annot>> endobj 4 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 15. Faltermeier, D. et al. Bandwidth-controlled Mott transition in -\(BEDT-TTF\)\ 2Cu[N\(CN\)2]BrxCl1 x: optical studies of localized charge excitations. \nPhys. Rev. B 76, 165113 \(2007\).\r:2518\ )/F 4/H/N/Rect[263.226 76.2059 268.431 63.6602]/Subtype/Link/Type/Annot>> endobj 5 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 16. Dressel, M. et al. Lattice vibrations of the charge-transfer salt  -\(BEDT-TTF\ \)2Cu2\(CN\)3: comprehensive explanation of the electrodynamic response in a spin-liquid compound. Phys. Rev. B 93, 081\ 201 \(2016\).\r:2519)/F 4/H/N/Rect[501.734 716.706 506.939 704.16]/Subtype/Link/Type/Annot>> endobj 6 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compounds\ . a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the intrins\ ic Mott physics is the Mott Hubbard b:2520)/F 4/H/N/Rect[418.853 695.706 436.457 683.16]/Subtype/Link/Type/Annot>> endobj 7 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compound\ s. a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the intrin\ sic Mott physics is the Mott Hubbard :2521)/F 4/H/N/Rect[424.062 674.706 433.437 662.16]/Subtype/Link/Type/Annot>> endobj 8 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 1 | Theoretical phase diagram of the Mott insulator. a, The boundary\ of the Mott state with a gapped density of states \(DOS\) manifests as a first-order transition below the critical endpoint and \ as the quantum Widom line above. Th:2522)/F 4/H/N/Rect[469.149 674.706 477.695 662.16]/Subtype/Link/Type/Annot>> endobj 9 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compoun\ ds. a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the intri\ nsic Mott physics is the Mott Hubbard:2523)/F 4/H/N/Rect[417.901 643.327 427.331 630.66]/Subtype/Link/Type/Annot>> endobj 10 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 11. Shimizu, Y. et al. Pressure-Tuned Exchange Coupling of a Quantum Spin Liquid i\ n the Molecular Triangular Lattice " \(ET\)2Ag2\(CN\)3. Phys. Rev. Lett. 117, 107203 \(2016\).\r:2524)/F 4/H/N/Rect[495.032 632.706 500.237 620.16]/Subtype/Link/Type/Annot>> endobj 11 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 17. Kandpal, H. C., Opahle, I., Zhang, Y.-Z., Jeschke, H. O. & Valent, R. Revisio\ n of model parameters for -type charge transfer salts: an ab initio Study. \nPhys. Rev. Lett. 103, 067004 \(2009\).\r:2525\ )/F 4/H/N/Rect[501.473 632.706 506.678 620.16]/Subtype/Link/Type/Annot>> endobj 12 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 18. Kato, R. & Hengbo, C. Cation dependence of crystal structure and \nband paramet\ ers in a series of molecular conductors,  2 -\(Cation\)\n[Pd\(dmit\)2]2 \(dmit: 1,3-dithiole-2-thione-4,5-dithiolate\). Cryst\ als 2, \n861 874 \(2012\).\r:2526)/F 4/H/N/Rect[507.914 632.706 513.119 620.16]/Subtype/Link/Type/Annot>> endobj 13 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 19. Furukawa, T., Miyagawa, K., Taniguchi, H., Kato, R. & Kanoda, K. \nQuantum crit\ icality of Mott transition in organic materials. Nat. Phys. 11, \n221 224 \(2015\).\r:2527)/F 4/H/N/Rect[346.165 559.206 351.37 546.66]/Subtype/Link/Type/Annot>> endobj 14 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compou\ nds. a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the intr\ insic Mott physics is the Mott Hubbar:2528)/F 4/H/N/Rect[356.206 548.706 377.8 536.16]/Subtype/Link/Type/Annot>> endobj 15 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 19. Furukawa, T., Miyagawa, K., Taniguchi, H., Kato, R. & Kanoda, K. \nQuantum cri\ ticality of Mott transition in organic materials. Nat. Phys. 11, \n221 224 \(2015\).\r:2529)/F 4/H/N/Rect[529.179 517.206 534.384 504.66]/Subtype/Link/Type/Annot>> endobj 16 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 3 | Correlation-dependent low-energy excitations. a c, While the \nlow-\ frequency conductivity is suppressed on cooling for EtMe \(c\) and AgCN \(b\), it increases for CuCN \(a\). d, The spectra\ l weight SW \(the integration range :2530)/F 4/H/N/Rect[365.411 402.32 369.875 388.277]/Subtype/Link/Type/Annot>> endobj 17 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 20. Nakamura, Y., Hiramatsu, T., Yoshida, Y., Saito, G. & Kishida, H. \nOptical pro\ perties of a quantum spin liquid candidate material, \n -\(BEDT-TTF\)2Ag2\(CN\)3. J. Phys. Soc. Jpn 86, 014710 \(2017\).\ \r:2531)/F 4/H/N/Rect[424.907 370.206 430.112 357.66]/Subtype/Link/Type/Annot>> endobj 18 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 3 | Correlation-dependent low-energy excitations. a c, While the \nlow\ -frequency conductivity is suppressed on cooling for EtMe \(c\) and AgCN \(b\), it increases for CuCN \(a\). d, The spectr\ al weight SW \(the integration range :2532)/F 4/H/N/Rect[434.689 360.32 443.235 346.277]/Subtype/Link/Type/Annot>> endobj 19 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 21. Kezsmarki, I. et al. Depressed charge gap in the triangular-lattice Mott insul\ ator " \(ET\)2Cu2\(CN\)3. Phys. Rev. B 74, 201101 \(2006\).\r:2533)/F 4/H/N/Rect[318.601 338.706 323.806 326.16]/Subtype/Link/Type/Annot>> endobj 20 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 3 | Correlation-dependent low-energy excitations. a c, While the \nlo\ w-frequency conductivity is suppressed on cooling for EtMe \(c\) and AgCN \(b\), it increases for CuCN \(a\). d, The spect\ ral weight SW \(the integration range :2534)/F 4/H/N/Rect[421.521 296.706 429.938 284.16]/Subtype/Link/Type/Annot>> endobj 21 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL compo\ unds. a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the int\ rinsic Mott physics is the Mott Hubba:2536)/F 4/H/N/Rect[537.988 265.206 547.418 252.66]/Subtype/Link/Type/Annot>> endobj 22 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 1 | Theoretical phase diagram of the Mott insulator. a, The boundar\ y of the Mott state with a gapped density of states \(DOS\) manifests as a first-order transition below the critical endpoint and\ as the quantum Widom line above. T:2537)/F 4/H/N/Rect[396.023 223.206 405.211 210.66]/Subtype/Link/Type/Annot>> endobj 23 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 3 | Correlation-dependent low-energy excitations. a c, While the \nl\ ow-frequency conductivity is suppressed on cooling for EtMe \(c\) and AgCN \(b\), it increases for CuCN \(a\). d, The spec\ tral weight SW \(the integration range :2538)/F 4/H/N/Rect[324.18 202.206 333.554 189.66]/Subtype/Link/Type/Annot>> endobj 24 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 19. Furukawa, T., Miyagawa, K., Taniguchi, H., Kato, R. & Kanoda, K. \nQuantum cr\ iticality of Mott transition in organic materials. Nat. Phys. 11, \n221 224 \(2015\).\r:2539)/F 4/H/N/Rect[338.706 191.706 343.911 179.16]/Subtype/Link/Type/Annot>> endobj 25 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 5. Vu\ri\revi, J., Terletska, H., Tanaskovi, D. & Dobrosavljevi, V. Finite-te\ mperature crossover and the quantum Widom line near the Mott transition. Phys. Rev. B 88, 075143 \(2013\).\r:2540)/F 4/H/N/Rect[320.684 160.206 323.286 147.66]/Subtype/Link/Type/Annot>> endobj 26 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 22. Terletska, H., Vu\ri\revi, J., Tanaskovi, D. & Dobrosavljevi, V. \nQuantum cr\ itical transport near the Mott transition. Phys. Rev. Lett. 107, \n026401 \(2011\).\r:2541)/F 4/H/N/Rect[324.522 160.206 329.727 147.66]/Subtype/Link/Type/Annot>> endobj 27 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 21. Kezsmarki, I. et al. Depressed charge gap in the triangular-lattice Mott insu\ lator " \(ET\)2Cu2\(CN\)3. Phys. Rev. B 74, 201101 \(2006\).\r:2542)/F 4/H/N/Rect[424.738 118.206 429.943 105.66]/Subtype/Link/Type/Annot>> endobj 28 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 19. Furukawa, T., Miyagawa, K., Taniguchi, H., Kato, R. & Kanoda, K. \nQuantum c\ riticality of Mott transition in organic materials. Nat. Phys. 11, \n221 224 \(2015\).\r:2543)/F 4/H/N/Rect[411.445 107.706 416.65 95.1602]/Subtype/Link/Type/Annot>> endobj 29 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 23. Pinteri, M. et al. Anisotropic charge dynamics in the spin-liquid candidate \n\  -\(BEDT-TTF\)2Cu2\(CN\)3. Phys. Rev. B 90, 195139 \(2014\).\r:2544)/F 4/H/N/Rect[528.814 55.2059 534.019 42.6602]/Subtype/Link/Type/Annot>> endobj 30 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 25. Lazi, P. et al. Importance of van der Waals interactions and \ncation anion co\ upling in an organic quantum spin liquid. Phys. Rev. B 97, 245134 \(2018\).\r:2545)/F 4/H/N/Rect[536.839 55.2059 542.043 42.6602]/Subtype/Link/Type/Annot>> endobj 31 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 5. Vu\ri\revi, J., Terletska, H., Tanaskovi, D. & Dobrosavljevi, V. Finite-tem\ perature crossover and the quantum Widom line near the Mott transition. Phys. Rev. B 88, 075143 \(2013\).\r:2510)/F 4/H/N/Rect[77.8472 291.556 80.3378 281.316]/Subtype/Link/Type/Annot>> endobj 32 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 33. Pustogow, A. Unveiling Electronic Correlations in Layered Molecular Conductors b\ y Optical Spectroscopy. 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Phys. 11, \n221 224 \(2015\).\r:2555)/F 4/H/N/Rect[93.6199 466.023 97.9247 455.784]/Subtype/Link/Type/Annot>> endobj 163 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 1 | Theoretical phase diagram of the Mott insulator. a, The bounda\ ry of the Mott state with a gapped density of states \(DOS\) manifests as a first-order transition below the critical endpoint an\ d as the quantum Widom line above. :2556)/F 4/H/N/Rect[167.35 403.023 174.102 392.784]/Subtype/Link/Type/Annot>> endobj 164 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 3 | Correlation-dependent low-energy excitations. a c, While the \n\ low-frequency conductivity is suppressed on cooling for EtMe \(c\) and AgCN \(b\), it increases for CuCN \(a\). d, The spe\ ctral weight SW \(the integration range:2557)/F 4/H/N/Rect[196.942 392.523 201.126 382.284]/Subtype/Link/Type/Annot>> endobj 165 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 33. Pustogow, A. Unveiling Electronic Correlations in Layered Molecular Conductor\ s by Optical Spectroscopy. 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Furukawa, T., Miyagawa, K., Taniguchi, H., Kato, R. & Kanoda, K. \nQuant\ um criticality of Mott transition in organic materials. Nat. Phys. 11, \n221 224 \(2015\).\r:2577)/F 4/H/N/Rect[236.793 167.627 240.991 157.509]/Subtype/Link/Type/Annot>> endobj 346 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 41. Georges, A., Kotliar, G., Krauth, W. & Rozenberg, M. J. Dynamical mean-field t\ heory of strongly correlated fermion systems and the limit of infinite dimensions. Rev. Mod. Phys. 68, 13 125 \(1996\).\r:25\ 78)/F 4/H/N/Rect[127.253 114.789 131.451 104.409]/Subtype/Link/Type/Annot>> endobj 347 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 42. Haule, K. Quantum Monte Carlo impurity solver for cluster dynamical mean-field\ theory and electronic structure calculations with adjustable cluster base. Phys. Rev. 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Phys. 68, 13 125 \(1996\).\r:2\ 581)/F 4/H/N/Rect[522.745 633.783 526.942 623.665]/Subtype/Link/Type/Annot>> endobj 350 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 2 | Temperature evolution of the optical conductivity of three QSL comp\ ounds. a c, The dominant feature in EtMe \(a\), AgCN \(b\) and CuCN \(c\) that contains all the information of the in\ trinsic Mott physics is the Mott Hubb:2582)/F 4/H/N/Rect[494.921 539.463 498.535 529.345]/Subtype/Link/Type/Annot>> endobj 351 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd:Fig. 1 | Theoretical phase diagram of the Mott insulator. a, The bound\ ary of the Mott state with a gapped density of states \(DOS\) manifests as a first-order transition below the critical endpoint a\ nd as the quantum Widom line above.:2583)/F 4/H/N/Rect[319.155 504.663 326.047 494.545]/Subtype/Link/Type/Annot>> endobj 352 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 5. Vu\ri\revi, J., Terletska, H., Tanaskovi, D. & Dobrosavljevi, V. Finite-\ temperature crossover and the quantum Widom line near the Mott transition. Phys. Rev. B 88, 075143 \(2013\).\r:2584)/F 4/H/N/Rect[469.07 487.758 471.169 476.433]/Subtype/Link/Type/Annot>> endobj 353 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 22. Terletska, H., Vu\ri\revi, J., Tanaskovi, D. & Dobrosavljevi, V. \nQuantum c\ ritical transport near the Mott transition. Phys. Rev. Lett. 107, \n026401 \(2011\).\r:2585)/F 4/H/N/Rect[472.165 487.758 476.363 476.433]/Subtype/Link/Type/Annot>> endobj 354 0 obj <>/BS<>/Border[0 0 0]/Dest(SpringerNature_NatMater_140.indd: 5. Vu\ri\revi, J., Terletska, H., Tanaskovi, D. & Dobrosavljevi, V. Finite\ -temperature crossover and the quantum Widom line near the Mott transition. Phys. Rev. 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Materials, doi:10.1038/s41563-018-0140-3 Quantum spin liquids unveil the genuine Mott state A. Pustogow M. Bories A. Lamp#x000F6;hle R. Ramp#x000F6;sslhuber E. Zhukova B. Gorshunov S. Tomiamp#x00107; J. A. Schlueter R. Hamp#x000FC;bner T. Hiramatsu Y. Yoshida G. Saito R. Kato T.-H. Lee V. Dobrosavljeviamp#x00107; S. Fratini M. 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