AuX (X=O, S)低电子态的理论研究

doi:10.3866/PKU.WHXB201405302

Abstract

Abstract:

Multireference approaches have commonly been employed to calculate low-lying states of openshell molecules with spin-orbit coupling (SOC), such as for AuO and AuS. However, by choosing a proper reference state, the equation-of-motion coupled-cluster approach (EOM-CC) can also be used to calculate some low-lying states of these molecules. Furthermore, the EOM-CC approach is a single-reference method and, therefore, more easily employed than multireference approaches. In this work, low-lying states of AuO and AuS are investigated based on a recently developed EOM-CC approach for ionization potentials (EOMIP-CC) with SOC at the CCSD level, using the corresponding anions as reference. The contribution of triples with EOMIPCC is estimated by comparing results of EOMIP-CCSD and EOMIP-CCSDT at a scalar relativistic level. In addition, compared with the EOMIP-CCSDT results, errors by UCCSD(T) can reach 0.1-0.15 eV when spin contamination is significant and the norm of T₁ is sizeable. When SOC is present, bond lengths and harmonic frequencies obtained with EOMIP-CCSD for the investigated states are in reasonable agreement with experimental data. Furthermore, ionization energies corresponding to the high-lying ²Δ_3/2, ²Σ_1/2⁺, and ²Π_1/2 states are overestimated by EOMIP-SOC-CCSD, but results for the other low- lying states agree well with the experimental data, with an error of approximately 0.2 eV. These results indicate that the single-reference EOMIPCCSD method with SOC is able to provide a reasonable description of low-lying states of AuO and AuS.

Key words: Spin-orbit coupling, Equation-of-motion coupled-cluster approach, Ionization energy

MSC2000:

O641

LIANG Yan-Ni, WANG Fan. Theoretical Studies on Low-Lying States of AuX (X=O, S)[J].Acta Phys. -Chim. Sin., 2014, 30(8): 1447-1455.

References

(1) Pitzer, K. S. Accounts Chem. Res. 1979, 12, 272.
(2) Pyykko, P.; Desclaux, J. P. Accounts Chem. Res. 1979, 12, 276. doi: 10.1021/ar50140a002
(3) Pyykko, P. Chem. Rev. 1988, 88, 563. doi: 10.1021/cr00085a006
(4) Love, J. C.; Estroff, L. A.; Kriebel, J. K.; Nuzzo, R. G.; Whitesides, G. M. Chem. Rev. 2005, 105, 1103. doi: 10.1021/cr0300789
(5) Griffiths, M. J.; Barrow, R. F. J. Chem. Soc., Faraday Trans. 1977, 73, 943. doi: 10.1039/f29777300943
(6) Citra, A.; Andrews, L. Theochem 1999, 489, 95. doi: 10.1016/S0166-1280(98)00516-8
(7) Sun, Q.; Jena, P.; Kim, Y. D.; Fischer, M.; Gantefor, G. J. Chem. Phys. 2004, 120, 6510. doi: 10.1063/1.1666009
(8) Ichino, T.; Gianola, A. J.; Andrews, D. H.; Lineberger,W. C. J. Phys. Chem. A 2004, 108, 11307. doi: 10.1021/jp045791w
(9) O'Brien, L. C.; Hardimon, S. C.; O'Brien, J. J. J. Phys. Chem. A 2004, 108, 11302. doi: 10.1021/jp045812m
(10) O′Brien, L. C.; Oberlink, A. E.; Roos, B. O. J. Phys. Chem. A 2006, 110, 11954. doi: 10.1021/jp063394a
(11) Okabayashi, T.; Koto, F.; Tsukamoto, K.; Yamazaki, E.; Tanimoto, M. Chem. Phys. Lett. 2005, 403, 223. doi: 10.1016/j.cplett.2005.01.003
(12) Zhai, H. J.; Bürgel, C.; Bonacic-Koutecky, V.;Wang, L. S. J. Am. Chem. Soc. 2008, 130, 9156. doi: 10.1021/ja802408b
(13) Legge, F. S.; Nyberg, G. L.; Peel, J. B. J. Phys. Chem. A 2001, 105, 790.
(14) Wu, Z. J. J. Phys. Chem. A 2005, 109, 5951. doi: 10.1021/jp0500283
(15) Yao, C.; Guan,W.; Song, P.; Su, Z. M.; Feng, J. D.; Yan, L. K.; Wu, Z. J. Theor. Chem. Acc. 2007, 117, 115.
(16) Becke, A. D. Phys. Rev. A 1988, 38, 3098. doi: 10.1103/PhysRevA.38.3098
(17) Perdew, J. P. Phys. Rev. B 1986, 33, 8822. doi: 10.1103/PhysRevB.33.8822
(18) Lee, C.; Yang,W.; Parr, R. G. Phys. Rev. B 1988, 37, 785. doi: 10.1103/PhysRevB.37.785
(19) Roos, B. O.; Malmqvist, P. Å. Phys. Chem. Chem. Phys. 2004, 6, 2919. doi: 10.1039/b401472n
(20) Li, Z.; Suo, B.; Zhang, Y.; Xiao, Y.; Liu,W. Mol. Phys. 2013, 111, 3741. doi: 10.1080/00268976.2013.785611
(21) Krylov, A. I. Annu. Rev. Phys. Chem. 2008, 59, 433. doi: 10.1146/annurev.physchem.59.032607.093602
(22) Stanton, J. F.; Gauss, J. J. Chem. Phys. 1994, 101, 8938. doi: 10.1063/1.468022
(23) Nooijen, M.; Bartlett, R. J. J. Chem. Phys. 1995, 102, 3629. doi: 10.1063/1.468592
(24) Tu, Z. Y.;Wang, F.; Li, X. Y. J. Chem. Phys. 2012, 136, 174102. doi: 10.1063/1.4704894
(25) Wang, F.; Gauss, J.; van Wüllen, C. J. Chem. Phys. 2008, 129, 064113. doi: 10.1063/1.2968136
(26) Kim, I.; Park, Y. C.; Kim, H.; Lee, Y. S. Chem. Phys. 2012, 395, 115. doi: 10.1016/j.chemphys.2011.05.002
(27) Cao, Z. L.;Wang, Z. F.; Yang, M. L.;Wang, F. Acta Phys. -Chim. Sin. 2014, 30 (3), 431. [曹战利, 王治钒, 杨明理, 王繁. 物理化学学报, 2014, 30 (3), 431.]. doi: 10.3866/PKU.WHXB201401023
(28) Liang, Y. N.;Wang, F.; Li, X. Y. Phys. Chem. Chem. Phys. 2013, 15, 17929. doi: 10.1039/c3cp52192c
(29) Stanton, J. F.; Gauss, J. J. Chem. Phys. 1999, 111, 8785. doi: 10.1063/1.479673
(30) Manohar, P. U.; Stanton, J. F.; Krylov, A. I. J. Chem. Phys. 2009, 131, 114112. doi: 10.1063/1.3231133
(31) Purvis, G. D., III; Bartlett, R. J. J. Chem. Phys. 1982, 76, 1910.
(32) Wang, F.; Gauss, J. J. Chem. Phys. 2008, 129, 174110. doi: 10.1063/1.3000010
(33) Wang, F.; Gauss, J. J. Chem. Phys. 2009, 131, 164113. doi: 10.1063/1.3245954
(34) Stanton, J. F.; Bartlett, R. J. J. Chem. Phys. 1993, 98, 7029. doi: 10.1063/1.464746
(35) Dolg, M.; Cao, X. Chem. Rev. 2011, 112, 403.
(36) Schwerdtfeger, P. ChemPhysChem 2011, 12, 3143. doi: 10.1002/cphc.201100387
(37) Figgen, D.; Rauhut, G.; Dolg, M.; Stoll, H. Chem. Phys. Lett. 2005, 311, 227.
(38) Weigend, F.; Baldes, A. J. Chem. Phys. 2010, 133, 174102. doi: 10.1063/1.3495681
(39) Rappoport, D.; Furche, F. J. Chem. Phys. 2010, 133, 134105. doi: 10.1063/1.3484283
(40) Stanton, J. F.; Gauss, J.; Harding, M. E.; Szalay, P. G.; Auer, A. A.; Bartlett, R. J.; Benedikt, U.; Berger, C.; Bernholdt, D. E.; Bomble, Y. J.; Cheng, L.; Christiansen, O.; Heckert, M.; Heun, O.; Huber, C.; Jagau, T. C.; Jonsson, D.; Jusélius, J.; Klein, K.; Lauderdale,W. J.; Matthews, D. A.; Metzroth, T.; Mück, L. A.; O’Neill, D. P.; Price, D. R.; Prochnow, E.; Puzzarini, C.; Ruud, K.; Schiffmann, F.; Schwalbach,W.; Stopkowicz, S.; Tajti, A.; Vázquez, J.;Wang, F.;Watts, J. D. and the integral packages MOLECULE (Almlöf, J.; Taylor, P. R.), PROPS (Taylor, P. R.), ABACUS (Helgaker, T.; Jensen, H. J. A.; Jørgensen, P.; Olsen, J.), and ECP routines by Mitin, A. V. and van Wüllen, C., CFOUR, Version 1.2; see http://www.cfour.de
(41) Liu,W. J.; van Wüllen, C. J. Chem. Phys. 1999, 110, 3730. doi: 10.1063/1.478237
(42) Seminario, J. M.; Zacarias, A. G.; Tour, J. M. J. Am. Chem. Soc. 1999, 121, 411. doi: 10.1021/ja982234c

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Theoretical Studies on Low-Lying States of AuX (X=O, S)

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