等电子三原子铀化物OUO<sup>2+</sup>、NUN和NUO<sup>+</sup>的结构和谐振频率的CCSD(T)计算研究

引用本文: 涂喆研, 杨冬冬, 王繁, 李象远. 等电子三原子铀化物OUO²⁺、NUN和NUO⁺的结构和谐振频率的CCSD(T)计算研究[J]. 物理化学学报, 2012, 28(07): 1707-1713. doi: 10.3866/PKU.WHXB201205111 shu

Citation: TU Zhe-Yan, YANG Dong-Dong, WANG Fan, LI Xiang-Yuan. A CCSD(T) Study on Structures and Harmonic Frequencies of the Isoelectronic Uranium Triatomic Species OUO²⁺, NUN and NUO⁺[J]. Acta Physico-Chimica Sinica, 2012, 28(07): 1707-1713. doi: 10.3866/PKU.WHXB201205111 shu

等电子三原子铀化物OUO²⁺、NUN和NUO⁺的结构和谐振频率的CCSD(T)计算研究

基金项目:
国家自然科学基金(20973116)资助项目 (20973116)

摘要:

用小核相对论有效势和CCSD(T)方法计算了三原子铀化物OUO²⁺, NUN和NUO⁺的平衡键长和谐振频率. 计算结果显示U原子内层5s5p5d 电子相关能对这些化合物性质的影响非常小. 除NUN的弯曲振动频率,旋轨耦合效应对这些化合物的结构和频率的影响并不明显. 本文的计算结果与其他研究组的计算结果以及已有的实验值相比符合较好, 这表明作为单参考态方法, CCSD(T)能够对这些体系的键长和频率给出较精确的计算结果. 与此前密度泛函理论(DFT)的计算结果相比, CCSD(T)方法与PBE0泛函的结果吻合最好. 本文的工作有助于在用密度泛函方法研究这些体系时选择合适的交换相关泛函, 也为今后的实验研究提供了新的理论数据.

关键词:

铀化物
/ 耦合簇理论
/ 旋轨耦合

English

A CCSD(T) Study on Structures and Harmonic Frequencies of the Isoelectronic Uranium Triatomic Species OUO²⁺, NUN and NUO⁺

1.
1. College of Chemistry, Sichuan University, Chengdu 610064, P. R. China;
2. College of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China
Received Date: 15 March 2012
Available Online: 07 June 2012
Fund Project:
国家自然科学基金(20973116)资助项目

Abstract:

CCSD(T) calculations with small-core relativistic effective core potentials for equilibrium bond lengths and harmonic frequencies are presented for uranium triatomic OUO²⁺, NUN, and NUO⁺ species. The inner shell electron correlation of the U atom has almost no effect on the properties of these species, and the spin-orbit coupling only has a small effect, except in the bending mode of NUN. Our results agree reasonably well with previous theoretical results and the available experimental data, which indicates that the single-reference CCSD(T) method can be employed to study these species. Compared with previous results, the CCSD(T) results agree best with density functional theory (DFT) calculations performed using the PBE0 functional. The present work provides new estimates which are useful for future experimental work and for choosing proper exchange-correlation functionals in DFT calculations for these species.

Key words:

1. [1]
  
  (1) Gabelnick, D.; Reedy, G. T.; Chasanov, M. G. J. Chem. Phys.1973, 58, 4468. doi: 10.1063/1.1679009
  (1) Gabelnick, D.; Reedy, G. T.; Chasanov, M. G. J. Chem. Phys.1973, 58, 4468. doi: 10.1063/1.1679009
2. [2]
  (2) Green, D.W.; Reedy, G. T. J. Chem. Phys. 1976, 65, 2921. doi: 10.1063/1.433406(2) Green, D.W.; Reedy, G. T. J. Chem. Phys. 1976, 65, 2921. doi: 10.1063/1.433406
3. [3]
  (3) Hunt, R. D.; Andrews, L. J. Chem. Phys. 1993, 98, 3690. doi: 10.1063/1.464045(3) Hunt, R. D.; Andrews, L. J. Chem. Phys. 1993, 98, 3690. doi: 10.1063/1.464045
4. [4]
  (4) Hunt, R. D.; Yustein, J. T.; Andrews, L. J. Chem. Phys. 1993,98, 6070. doi: 10.1063/1.464845(4) Hunt, R. D.; Yustein, J. T.; Andrews, L. J. Chem. Phys. 1993,98, 6070. doi: 10.1063/1.464845
5. [5]
  (5) Pyykkö, P. Chem. Rev. 1988, 88, 563. doi: 10.1021/cr00085a006(5) Pyykkö, P. Chem. Rev. 1988, 88, 563. doi: 10.1021/cr00085a006
6. [6]
  (6) Pepper, M.; Bursten, B. E. Chem. Rev. 1991, 91, 719. doi: 10.1021/cr00005a005(6) Pepper, M.; Bursten, B. E. Chem. Rev. 1991, 91, 719. doi: 10.1021/cr00005a005
7. [7]
  (7) Cornehl, H. H.; Heinemann, C.; Marcalo, J.; de Matos, A. P.;Schwarz, H. Angew. Chem. Int. Edit. 1996, 35, 891. doi: 10.1002/anie.199608911(7) Cornehl, H. H.; Heinemann, C.; Marcalo, J.; de Matos, A. P.;Schwarz, H. Angew. Chem. Int. Edit. 1996, 35, 891. doi: 10.1002/anie.199608911
8. [8]
  (8) Zhou, M.; Andrews, L. J. Chem. Phys. 1996, 111, 11044.(8) Zhou, M.; Andrews, L. J. Chem. Phys. 1996, 111, 11044.
9. [9]
  (9) Dolg, M. Effective Core Potentials. In Modern Methods and Al rithms of Quantum Chemistry; Grotendorst, J. Ed.; JohnNeumann Institute for Computing: Jülich, 2000; Vol. 3, p 507.(9) Dolg, M. Effective Core Potentials. In Modern Methods and Al rithms of Quantum Chemistry; Grotendorst, J. Ed.; JohnNeumann Institute for Computing: Jülich, 2000; Vol. 3, p 507.
10. [10]
  (10) Pyykkö, P.; Li, J.; Runeberg, N. J. Phys. Chem. 1994, 98, 4809.doi: 10.1021/j100069a007(10) Pyykkö, P.; Li, J.; Runeberg, N. J. Phys. Chem. 1994, 98, 4809.doi: 10.1021/j100069a007
11. [11]
  (11) Gagliardi, L.; Roos, B. O. Chem. Phys. Lett. 2000, 331, 229.doi: 10.1016/S0009-2614(00)01218-5(11) Gagliardi, L.; Roos, B. O. Chem. Phys. Lett. 2000, 331, 229.doi: 10.1016/S0009-2614(00)01218-5
12. [12]
  (12) de Jong,W. A.; Harrison, R. J.; Nichols, J. A.; Dixon, D. A.Theor. Chem. Acc. 2001, 107, 22. doi: 10.1007/s002140100293(12) de Jong,W. A.; Harrison, R. J.; Nichols, J. A.; Dixon, D. A.Theor. Chem. Acc. 2001, 107, 22. doi: 10.1007/s002140100293
13. [13]
  (13) Wang, H. Y.; Chen, C. A.; Sun, Y.; Zhu, Z. H. Acta Phys. -Chim. Sin. 2003, 19, 651. [王红艳, 陈长安, 孙颖, 朱正和. 物理化学学报, 2003, 19, 651.] doi: 10.3866/PKU.WHXB20030717(13) Wang, H. Y.; Chen, C. A.; Sun, Y.; Zhu, Z. H. Acta Phys. -Chim. Sin. 2003, 19, 651. [王红艳, 陈长安, 孙颖, 朱正和. 物理化学学报, 2003, 19, 651.] doi: 10.3866/PKU.WHXB20030717
14. [14]
  (14) Clavaguéra-Sarrio, C.; Ismail, N.; Marsden, C. J.; Bégué, D.;Pouchan, C. Chem. Phys. 2004, 302, 1. doi: 10.1016/j.chemphys.2004.03.011(14) Clavaguéra-Sarrio, C.; Ismail, N.; Marsden, C. J.; Bégué, D.;Pouchan, C. Chem. Phys. 2004, 302, 1. doi: 10.1016/j.chemphys.2004.03.011
15. [15]
  (15) Czek, J. J. Chem. Phys. 1966, 45, 4256. doi: 10.1063/1.1727484(15) Czek, J. J. Chem. Phys. 1966, 45, 4256. doi: 10.1063/1.1727484
16. [16]
  (16) Jackson, V. E.; Craciun, R.; Dixon, D. A.; Peterson, K. A.; deJong,W. A. J. Phys. Chem. A 2008, 112, 4095. doi: 10.1021/jp710334b(16) Jackson, V. E.; Craciun, R.; Dixon, D. A.; Peterson, K. A.; deJong,W. A. J. Phys. Chem. A 2008, 112, 4095. doi: 10.1021/jp710334b
17. [17]
  (17) Stanton, J. F.; Gauss, J.; Harding, M. E.; Szalay, P. G. withcontributions from 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. and Taylor, P. R.), PROPS (Taylor, P. R.), ABACUS (Helgaker, T.; Jensen, H. J. A.; Jørgensen, P. and Olsen, J.), andECP routines by Mitin, A. V. and vanWüllen, C.; CFOUR,Version1.2; For the current version, see http://www.cfour.de.(17) Stanton, J. F.; Gauss, J.; Harding, M. E.; Szalay, P. G. withcontributions from 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. and Taylor, P. R.), PROPS (Taylor, P. R.), ABACUS (Helgaker, T.; Jensen, H. J. A.; Jørgensen, P. and Olsen, J.), andECP routines by Mitin, A. V. and vanWüllen, C.; CFOUR,Version1.2; For the current version, see http://www.cfour.de.
18. [18]
  (18) Wang, F.; Gauss, J.; van Wüllen, C. J. Chem. Phys. 2008, 129,064113. doi: 10.1063/1.2968136(18) Wang, F.; Gauss, J.; van Wüllen, C. J. Chem. Phys. 2008, 129,064113. doi: 10.1063/1.2968136
19. [19]
  (19) Wang, F.; Gauss, J. J. Chem. Phys. 2008, 129, 174110. doi: 10.1063/1.3000010(19) Wang, F.; Gauss, J. J. Chem. Phys. 2008, 129, 174110. doi: 10.1063/1.3000010
20. [20]
  (20) Wang, F.; Gauss, J. J. Chem. Phys. 2009, 131, 164113. doi: 10.1063/1.3245954(20) Wang, F.; Gauss, J. J. Chem. Phys. 2009, 131, 164113. doi: 10.1063/1.3245954
21. [21]
  (21) Kuechle,W.; Dolg, M.; Stoll, H.; Preuss, H. J. Chem. Phys.1994, 100, 7535. doi: 10.1063/1.466847(21) Kuechle,W.; Dolg, M.; Stoll, H.; Preuss, H. J. Chem. Phys.1994, 100, 7535. doi: 10.1063/1.466847
22. [22]
  (22) Cao, X.; Dolg, M.; Stoll, H. J. Chem. Phys. 2003, 118, 487. doi: 10.1063/1.1521431(22) Cao, X.; Dolg, M.; Stoll, H. J. Chem. Phys. 2003, 118, 487. doi: 10.1063/1.1521431
23. [23]
  (23) Cao, X.; Dolg, M. J. Mol. Struct. -Theochem 2004, 673, 203.doi: 10.1016/j.theochem.2003.12.015(23) Cao, X.; Dolg, M. J. Mol. Struct. -Theochem 2004, 673, 203.doi: 10.1016/j.theochem.2003.12.015
24. [24]
  (24) Kendall, R. A.; Dunning, T. H.; Harrison, R. J. J. Chem. Phys.1992, 96, 6796. doi: 10.1063/1.462569(24) Kendall, R. A.; Dunning, T. H.; Harrison, R. J. J. Chem. Phys.1992, 96, 6796. doi: 10.1063/1.462569
25. [25]
  (25) te Velde, G.; Bickelhaupt, F. M.; Baerends, E. J.; FonsecaGuerra, C.; van Gisbergen, S. J. A.; Snijders, J. G.; Ziegler, T.J. Comput. Chem. 2001, 22, 931. doi: 10.1002/jcc.1056(25) te Velde, G.; Bickelhaupt, F. M.; Baerends, E. J.; FonsecaGuerra, C.; van Gisbergen, S. J. A.; Snijders, J. G.; Ziegler, T.J. Comput. Chem. 2001, 22, 931. doi: 10.1002/jcc.1056
26. [26]
  (26) Becke, A. D. Phys. Rev. A 1988, 38, 3098. doi: 10.1103/PhysRevA.38.3098(26) Becke, A. D. Phys. Rev. A 1988, 38, 3098. doi: 10.1103/PhysRevA.38.3098
27. [27]
  (27) Perdew, J. P. Phys. Rev. B 1986, 33, 8822. doi: 10.1103/PhysRevB.33.8822(27) Perdew, J. P. Phys. Rev. B 1986, 33, 8822. doi: 10.1103/PhysRevB.33.8822
28. [28]
  (28) Lee, T. J.; Taylor, P. R. Int. J. Quantum Chem. Symp. 1989, 23,199.(28) Lee, T. J.; Taylor, P. R. Int. J. Quantum Chem. Symp. 1989, 23,199.
29. [29]
  (29) Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.; Frisch, M. J.J. Phys. Chem. 1994, 98, 11623. doi: 10.1021/j100096a001(29) Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.; Frisch, M. J.J. Phys. Chem. 1994, 98, 11623. doi: 10.1021/j100096a001
30. [30]
  (30) Grimme, S. J. Comput. Chem. 2004, 25, 1463. doi: 10.1002/jcc.20078(30) Grimme, S. J. Comput. Chem. 2004, 25, 1463. doi: 10.1002/jcc.20078
31. [31]
  (31) Ernzerhof, M.; Scuseria, G. J. Chem. Phys. 1999, 110, 5029.doi: 10.1063/1.478401(31) Ernzerhof, M.; Scuseria, G. J. Chem. Phys. 1999, 110, 5029.doi: 10.1063/1.478401
32. [32]
  (32) Perdew, J. P.; Chevary, J. A.; Vosko, S. H.; Jackson, K. A.;Peterson, M. R.; Sing, D. J.; Fiolhais, C. Phys. Rev. B 1992, 46,6671. doi: 10.1103/PhysRevB.46.6671
  (32) Perdew, J. P.; Chevary, J. A.; Vosko, S. H.; Jackson, K. A.;Peterson, M. R.; Sing, D. J.; Fiolhais, C. Phys. Rev. B 1992, 46,6671. doi: 10.1103/PhysRevB.46.6671

扫一扫看文章

计量

PDF下载量: 607
文章访问数: 1789
HTML全文浏览量: 8

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

等电子三原子铀化物OUO²⁺、NUN和NUO⁺的结构和谐振频率的CCSD(T)计算研究

English

A CCSD(T) Study on Structures and Harmonic Frequencies of the Isoelectronic Uranium Triatomic Species OUO²⁺, NUN and NUO⁺

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

等电子三原子铀化物OUO2+、NUN和NUO+的结构和谐振频率的CCSD(T)计算研究

English

A CCSD(T) Study on Structures and Harmonic Frequencies of the Isoelectronic Uranium Triatomic Species OUO2+, NUN and NUO+

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

等电子三原子铀化物OUO²⁺、NUN和NUO⁺的结构和谐振频率的CCSD(T)计算研究

A CCSD(T) Study on Structures and Harmonic Frequencies of the Isoelectronic Uranium Triatomic Species OUO²⁺, NUN and NUO⁺

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs