Ab initio model potentials (AIMP) listed below were obtained in a self-consistent embedding ion (SCEI) calculation on the original Cs2ZrCl4 crystal.[1] The following computational details were used: ANO-RCC-VDZP for the main atoms and for the first coordinated ones Individual clusters were built for Cs, Zr and Cl ions, in which these elements are placed at the origin of the coordinates. Three layers of AIMP potentials accounted for the surrounding atoms. Ten layers of point charges simulated the remaining crystal: Cs = +1; Zr = +4; and Cl = -1; The obtained molecular orbitals and density of the central element were used to fit the AIMP potential for each element, and were used in the subsequent SCEI iteration. The entire procedure convergerged in about 12-15 SCEI iterations for all elements. The potentials listed below are in the format of Seward program in MOLCAS package[2]. Refs: [1] J. L. Pascual and L. Seijo, J. Chem. Phys., Vol. 102, No. 13, 1995. [2] F. Aquilante, J. Autschbach, R. K. Carlson, L. F. Chibotaru, M. G. Delcey, L. De Vico, I. Fdez. Galván, N. Ferré, L. M. Frutos, L. Gagliardi, M. Garavelli, A. Giussani, C. E. Hoyer, G. Li Manni, H. Lischka, D. Ma, P. Å. Malmqvist, T. Müller, A. Nenov, M. Olivucci, T. B. Pedersen, D. Peng, F. Plasser, B. Pritchard, M. Reiher, I. Rivalta, I. Schapiro, J. Segarra‐Martí, M. Stenrup, D. G. Truhlar, L. Ungur, A. Valentini, S. Vancoillie, V. Veryazov, V. P. Vysotskiy, O. Weingart, F. Zapata, R. Lindh, MOLCAS 8: New Capabilities for Multiconfigurational Quantum Chemical Calculations across the Periodic Table J. Comput. Chem., 37, 506-541, (2016); *========================================================================== Basis Set Zr.ECP.... / inline 4.000 0 0 0 M1 13 415880.0000 68978.00000 17179.00000 5050.200000 1646.960000 591.0000000 219.7100000 88.92000000 31.91000000 11.65220000 4.985000000 1.692400000 0.8301300000 0.7614898459E-01 0.8672984761E-01 0.1533183211 0.2663092845 0.4175371680 0.4748806701 0.7089122634 1.397846244 1.196345824 2.136178485 0.9626170034 0.9086778540 0.2144980510 M2 0 COREREP 1.000 PROJOP 2 13 4 2 2 2 2 1303.772105 184.7871230 33.39544607 5.835353241 22517.10490 3391.918900 768.9299900 207.1223170 309.5463010 35.21428790 14.98494400 27.52608110 4.734677850 2.109400820 3.440439540 0.6786342260 0.2947809880 -0.016718853671 -0.005827163430 0.002487862599 0.000963430935 -0.117626570681 -0.040997383225 0.017503517380 0.006778280331 -0.432262794143 -0.150660206471 0.064323216144 0.024909324300 -0.558441985029 -0.194638506728 0.083099413120 0.032180452947 0.002436669157 -0.109815137479 0.045268387792 0.015084954631 -0.014076722789 0.634405883025 -0.261517056661 -0.087146309541 -0.009340979836 0.420976718106 -0.173536524782 -0.057828226956 0.000645573762 0.099588538732 -0.409233599802 -0.205761127645 -0.002014052925 -0.310695074086 1.276721852013 0.641930985350 -0.000934687565 -0.144188277617 0.592504806778 0.297909206958 0.008655303399 0.414954551763 -0.538259740986 0.053056782887 -0.003562861579 0.013353865689 -0.076404497402 -1.166815563470 0.001855306187 -0.002269235728 0.031116884632 -0.165184415335 10 3 6 6 6 169.3199163 27.33867177 3.919234102 981.4297120 230.9750870 72.08684850 24.82378740 11.44808270 4.716449610 2.023746630 1.100792660 0.4804636130 0.1967857670 0.026375246312 0.008332379566 0.002894106556 0.173748626490 0.054890084736 0.019065112532 0.497839746991 0.157275867150 0.054627026361 0.461886145629 0.145917525705 0.050681904781 0.003870313941 0.260568948514 0.122330658867 0.006523741097 0.439210974613 0.206198659558 0.002324862056 0.156521375387 0.073482903804 0.004432387218 0.065894007362 0.431816767003 0.005027649630 0.042058545196 0.332584666525 0.001935896247 0.013822521554 0.034415235682 7 1 10 16.40644743 94.59558890 26.71735310 8.935796000 2.972978130 1.478689890 0.4818253610 0.1425757710 0.053422167121 0.279442695964 0.542855812012 0.366370392023 0.001326767768 0.020857435999 0.005518072697 Spectral Representation Operator Core primitive basis Exchange End of Spectral Representation Operator ... insert coordinates of the Zr4+ ... End of Basis Set *========================================================================== Basis Set Cl.ECP.... / Inline -1.000 0 0 0 M1 11 273400.0000 32560.00000 6397.000000 1584.700000 473.9000000 158.8100000 47.66000000 14.29200000 5.141000000 1.432600000 0.5005000000 -.1250983140 -.1839470459 -.3523551428 -.6687821944 -1.055427358 -1.432341694 -1.957390475 -4.392128198 -2.869010858 -2.272267635 -2.691251085 M2 0 COREREP 1.000 PROJOP 1 9 3 2 2 2 207.0420387 20.69149294 1.933700295 601.3455000 109.5358000 29.64481000 38.96043000 9.053550000 2.944501000 2.129386000 0.5940930000 0.2325240000 0.153781476336 -0.045374611348 0.013235398917 0.526269571493 -0.192999163434 0.057313823564 0.400202482871 -0.263352931869 0.081005308245 0.038422007126 -0.009964924967 0.004698182358 0.016052594958 0.345536375748 -0.123779108736 0.030250113728 0.861224407122 -0.528849145506 -0.025528267726 -0.086682030034 0.083444499015 0.004117768921 0.081783926982 0.329087192416 -0.001400585283 -0.021116345087 0.812597505468 6 2 6 6 15.59000270 0.7063387365 38.96043000 9.053550000 2.944501000 2.129386000 0.5940930000 0.2325240000 0.190085996322 0.040529388586 0.562364292769 0.119584574297 0.335782357287 0.179116313626 0.083932855651 0.162467302790 0.026189274583 0.277371443018 0.005108496575 0.541214095494 Spectral Representation Operator Core primitive basis Exchange End of Spectral Representation Operator ... insert coordinates of the Cl- ... End Of Basis Set *========================================================================== Basis Set Cs.ECP.... / inline 1.000 0 0 0 M1 15 442566.0000 75310.00000 19356.20000 5899.400000 1925.510000 611.9800000 228.4800000 79.45600000 32.10600000 17.87100000 4.632500000 2.124400000 0.7226200000 0.3647600000 0.1556550000 0.4719738527 0.5340455764 0.9059590487 1.534933699 2.204783072 2.853944491 6.268847746 3.291880147 11.21017747 2.679863778 11.94978995 3.407589231 4.628915853 2.030994472 0.2630162105E-01 M2 0 COREREP 1.000 PROJOP 1 11 5 2 2 2 2 2 2663.571540 425.8016310 92.04998600 19.03992570 2.397325627 33313.72970 3974.353370 773.5431020 68.95959780 23.82251990 14.68367750 7.100338070 4.198977640 1.836810800 0.3628488660 0.1568368940 0.051400731232 0.017713712496 0.007728950342 0.003475158893 0.001220915065 0.254359876061 0.106434067340 0.050184496802 0.023581409399 0.008539396664 0.736676609491 0.358208729607 0.168004099684 0.077418281567 0.029130335655 0.288025409682 -0.825579235015 -0.739489961625 -0.390942720883 -0.144594744385 -0.658799668730 -0.345777226928 -0.356661923265 -0.274413318564 -0.104256918485 0.786232365519 0.112218163553 0.926930016381 0.875777668192 0.341292683348 -0.543594818799 -0.040730461012 0.521270119723 0.686329463273 0.373986630842 0.304811674842 0.016739812040 0.050760226596 -0.429460146332 -0.300475052555 -0.067898881494 -0.003297786695 0.008617958744 -1.085791202739 -0.838227918542 0.013543212453 0.000210733999 -0.000991882440 -0.073917256406 0.900596030902 -0.006034411061 -0.000159447599 0.000496693802 0.023720667601 0.383573177007 10 4 6 6 6 6 381.9007070 77.53220420 14.19044920 1.165042561 1835.939350 412.7449050 125.9339220 18.54755560 8.381149310 4.592322460 2.150344150 0.4615536950 0.2062279720 0.9242510220E-01 0.056520125787 0.021686907394 0.009272738120 -0.002894662172 0.171899236514 0.111813193543 0.053187300783 -0.018924880043 0.737178558440 0.339659458519 0.151122413823 -0.050161383568 0.444446974330 -0.562858154294 -0.442982860886 0.152494202726 -0.460759081787 -0.485193638558 -0.216995649630 0.108815757151 0.324536875925 -0.003463784316 0.271144558213 -0.197323930739 -0.106213989013 -0.023768939091 0.842773248291 -0.362110442804 0.032403023471 0.005853287609 0.149950755473 0.515987949585 -0.024513628795 -0.004775439839 -0.078570531972 0.548427145154 0.008754292582 0.001732365898 0.025020547459 0.068446356669 Spectral Representation Operator Core primitive basis Exchange End of Spectral Representation Operator ... insert coordinates of the Cs+ ... End of Basis Set