水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

引用本文: 王友娟, 赵东波, 荣春英, 刘述斌. 水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究[J]. 物理化学学报, 2013, 29(10): 2173-2179. doi: 10.3866/PKU.WHXB201308272 shu

Citation: WANG You-Juan, ZHAO Dong-Bo, RONG Chun-Ying, LIU Shu-Bin. Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study[J]. Acta Physico-Chimica Sinica, 2013, 29(10): 2173-2179. doi: 10.3866/PKU.WHXB201308272 shu

水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

基金项目:
湖南师范大学&ldquo

潇湘学者&rdquo

杰出人才项目(23040609) (23040609)

湖南省研究生创新项目(CX2012B223)以及湖南省高等教育机构科技创新研究团队项目资助 (CX2012B223)

摘要:

寻找确定分子体系构象稳定性的关键因素是至关重要的, 但即使对最简单的分子, 其稳定性的起源和本质仍存在很大的争议. 本文以水团簇为例, 采用量子分子动力学产生185个八聚水分子团簇模型, 并运用基于密度泛函理论的两个能量分解方法寻找其稳定性的决定因素. 我们发现不同水团簇的稳定性与其立体排斥能和交换相关能成良好的线性关系.本文还采用双变量模型模拟水团簇的稳定性, 取得了更好的结果(相关系数大于0.99). 本工作对揭示包括水分子团簇在内的通过弱相互作用组成的分子络合物的稳定性起源和本质提供了有益启示.

关键词:

English

Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study

1.
1 Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research (Ministry of Education of China) and Key Laboratory of Resource Fine-Processing and Advanced Materials of Hunan Province, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, P. R. China;
2 Research Computing Center, University of North Carolina, Chapel Hill, North Carolina 27599-3420, U.S.A.
Received Date: 27 June 2013
Available Online: 26 September 2013
Fund Project:
湖南师范大学&ldquo

潇湘学者&rdquo

杰出人才项目(23040609)

湖南省研究生创新项目(CX2012B223)以及湖南省高等教育机构科技创新研究团队项目资助

Abstract:

To find out what interaction dictates the molecular stability is essential, yet still controversial even for simplest molecules. Here, using water cluster as an example, we employ quantum molecular dynamics to generate a total of 185 conformations for octamer water clusters and then employ two energy partition schemes from density functional theory to pinpoint the principles verning their stability. We found that their stability is strongly correlated with steric repulsion and exchange-correlation interactions. Explanations using two different quantities are also proposed (with the correlation coefficient larger than 0.99). This work sheds light to the fundamental understanding towards the origin and nature of molecular conformational stability for water clusters and other molecular complexes formed through intermolecular interactions.

Key words:

1. [1]
  
  (1) Liu, S. B. J. Phys. Chem. A 2013, 117, 962. doi: 10.1021/jp312521z
  (1) Liu, S. B. J. Phys. Chem. A 2013, 117, 962. doi: 10.1021/jp312521z
2. [2]
  (2) Pophristic, V.; odman, L. Nature 2001, 411, 565. doi: 10.1038/35079036(2) Pophristic, V.; odman, L. Nature 2001, 411, 565. doi: 10.1038/35079036
3. [3]
  (3) Bickelhaupt, F. M.; Baerends, E. J. Angew. Chem. Int. Edit.2003, 42, 4183.(3) Bickelhaupt, F. M.; Baerends, E. J. Angew. Chem. Int. Edit.2003, 42, 4183.
4. [4]
  (4) Weinhold, F. Angew. Chem. Int. Edit. 2003, 42, 4188.(4) Weinhold, F. Angew. Chem. Int. Edit. 2003, 42, 4188.
5. [5]
  (5) Mo, Y. R. Nat. Chem. 2010, 2, 666. doi: 10.1038/nchem.721(5) Mo, Y. R. Nat. Chem. 2010, 2, 666. doi: 10.1038/nchem.721
6. [6]
  (6) Mo, Y.; Gao, J. Accounts Chem. Res. 2007, 40, 113. doi: 10.1021/ar068073w(6) Mo, Y.; Gao, J. Accounts Chem. Res. 2007, 40, 113. doi: 10.1021/ar068073w
7. [7]
  (7) Parr, R. G.; Yang, W. Density Functional Theory of Atoms Molecules; Oxford University Press: NewYork, 1989.(7) Parr, R. G.; Yang, W. Density Functional Theory of Atoms Molecules; Oxford University Press: NewYork, 1989.
8. [8]
  (8) Geerlings, P.; De Proft, F.; Langenaeker, W. Chem. Rev. 2003,103, 1793. doi: 10.1021/cr990029p(8) Geerlings, P.; De Proft, F.; Langenaeker, W. Chem. Rev. 2003,103, 1793. doi: 10.1021/cr990029p
9. [9]
  (9) Liu, S. B. Acta Phys. -Chim. Sin. 2009, 25, 590. [刘述斌. 物理化学学报, 2009, 25, 590.] doi: 10.3866/PKU.WHXB20090332(9) Liu, S. B. Acta Phys. -Chim. Sin. 2009, 25, 590. [刘述斌. 物理化学学报, 2009, 25, 590.] doi: 10.3866/PKU.WHXB20090332
10. [10]
  (10) Levy, M.; Perdew, J. P. Phys. Rev. A 1985, 32, 2010. doi: 10.1103/PhysRevA.32.2010(10) Levy, M.; Perdew, J. P. Phys. Rev. A 1985, 32, 2010. doi: 10.1103/PhysRevA.32.2010
11. [11]
  (11) Liu, S. B.; Parr, R. G. Phys. Rev. A 1996, 53, 2211. doi: 10.1103/PhysRevA.53.2211(11) Liu, S. B.; Parr, R. G. Phys. Rev. A 1996, 53, 2211. doi: 10.1103/PhysRevA.53.2211
12. [12]
  (12) Liu, S. B.; Nagy, A.; Parr, R. G. Phys. Rev. A 1999, 59, 1131.doi: 10.1103/PhysRevA.59.1131(12) Liu, S. B.; Nagy, A.; Parr, R. G. Phys. Rev. A 1999, 59, 1131.doi: 10.1103/PhysRevA.59.1131
13. [13]
  (13) Liu, S. B.; Morrison, R. C.; Parr, R. G. J. Chem. Phys. 2006,125, 174109. doi: 10.1063/1.2378769(13) Liu, S. B.; Morrison, R. C.; Parr, R. G. J. Chem. Phys. 2006,125, 174109. doi: 10.1063/1.2378769
14. [14]
  (14) Liu, S. B. J. Chem. Phys. 2007, 126, 244103. doi: 10.1063/1.2747247(14) Liu, S. B. J. Chem. Phys. 2007, 126, 244103. doi: 10.1063/1.2747247
15. [15]
  (15) March, N. H. Phys. Lett. A 1986, 113, 476. doi: 10.1016/0375-9601(86)90123-4(15) March, N. H. Phys. Lett. A 1986, 113, 476. doi: 10.1016/0375-9601(86)90123-4
16. [16]
  (16) Holas, A.; March, N. H. Phys. Rev. A 1991, 44, 5521. doi: 10.1103/PhysRevA.44.5521(16) Holas, A.; March, N. H. Phys. Rev. A 1991, 44, 5521. doi: 10.1103/PhysRevA.44.5521
17. [17]
  (17) von Weizsäcker, C. F. Z. Phys. 1935, 96, 431. doi: 10.1007/BF01337700(17) von Weizsäcker, C. F. Z. Phys. 1935, 96, 431. doi: 10.1007/BF01337700
18. [18]
  (18) Weisskopf, V. F. Science 1975, 187, 605. doi: 10.1126/science.187.4177.605(18) Weisskopf, V. F. Science 1975, 187, 605. doi: 10.1126/science.187.4177.605
19. [19]
  (19) Liu, S. B. Phys. Rev. A 1996, 54, 4863. doi: 10.1103/PhysRevA.54.4863(19) Liu, S. B. Phys. Rev. A 1996, 54, 4863. doi: 10.1103/PhysRevA.54.4863
20. [20]
  (20) Liu, S. B.; Parr, R. G. Phys. Rev. A 1997, 55, 1792. doi: 10.1103/PhysRevA.55.1792(20) Liu, S. B.; Parr, R. G. Phys. Rev. A 1997, 55, 1792. doi: 10.1103/PhysRevA.55.1792
21. [21]
  (21) Tsirelson, V. G.; Stash, A. I.; Liu, S. B. J. Chem. Phys. 2010,133, 114110. doi: 10.1063/1.3492377(21) Tsirelson, V. G.; Stash, A. I.; Liu, S. B. J. Chem. Phys. 2010,133, 114110. doi: 10.1063/1.3492377
22. [22]
  (22) Liu, S. B. J. Chem. Phys. 2007, 126, 191107. doi: 10.1063/1.2741244(22) Liu, S. B. J. Chem. Phys. 2007, 126, 191107. doi: 10.1063/1.2741244
23. [23]
  (23) Esquivel, R. O.; Liu, S. B.; Angulo, J. C.; Dehesa, J. S.; Antolín,J.; Molina-Espíritu, M. J. Phys. Chem. A 2011, 115, 4406. doi: 10.1021/jp1095272(23) Esquivel, R. O.; Liu, S. B.; Angulo, J. C.; Dehesa, J. S.; Antolín,J.; Molina-Espíritu, M. J. Phys. Chem. A 2011, 115, 4406. doi: 10.1021/jp1095272
24. [24]
  (24) Liu, S. B.; vind, N. J. Phys. Chem. A 2008, 112, 6690. doi: 10.1021/jp800376a(24) Liu, S. B.; vind, N. J. Phys. Chem. A 2008, 112, 6690. doi: 10.1021/jp800376a
25. [25]
  (25) Liu, S. B.; vind, N.; Pedersen, L. G. J. Chem. Phys. 2008,129, 094104. doi: 10.1063/1.2976767(25) Liu, S. B.; vind, N.; Pedersen, L. G. J. Chem. Phys. 2008,129, 094104. doi: 10.1063/1.2976767
26. [26]
  (26) Liu, S. B.; Hu, H.; Pedersen, L. G. J. Phys. Chem. A 2010, 114,5913. doi: 10.1021/jp101329f(26) Liu, S. B.; Hu, H.; Pedersen, L. G. J. Phys. Chem. A 2010, 114,5913. doi: 10.1021/jp101329f
27. [27]
  (27) Ess, D. H.; Liu, S. B.; De Proft, F. J. Phys. Chem. A 2010, 114,12952. doi: 10.1021/jp108577g(27) Ess, D. H.; Liu, S. B.; De Proft, F. J. Phys. Chem. A 2010, 114,12952. doi: 10.1021/jp108577g
28. [28]
  (28) Huang, Y.; Zhong, A. G.; Yang, Q.; Liu, S. B. J. Chem. Phys.2011, 134, 084103. doi: 10.1063/1.3555760(28) Huang, Y.; Zhong, A. G.; Yang, Q.; Liu, S. B. J. Chem. Phys.2011, 134, 084103. doi: 10.1063/1.3555760
29. [29]
  (29) Zhao, D. B.; Rong, C. Y.; Jenkins, S.; Kirk, S. R.; Yin, D. L.;Liu, S. B. Acta Phys. -Chim. Sin. 2013, 29, 43. [赵东波, 荣春英,苏曼,苏文,尹笃林, 刘述斌.物理化学学报, 2013, 29,43.] doi: 10.3866/PKU.WHXB201211121(29) Zhao, D. B.; Rong, C. Y.; Jenkins, S.; Kirk, S. R.; Yin, D. L.;Liu, S. B. Acta Phys. -Chim. Sin. 2013, 29, 43. [赵东波, 荣春英,苏曼,苏文,尹笃林, 刘述斌.物理化学学报, 2013, 29,43.] doi: 10.3866/PKU.WHXB201211121
30. [30]
  (30) Tsirelson, V. G.; Stash, A. I.; Karasiev, V. V.; Liu, S. B. Comp. Theor. Chem. 2013, 1006, 92. doi: 10.1016/j.comptc.2012.11.015(30) Tsirelson, V. G.; Stash, A. I.; Karasiev, V. V.; Liu, S. B. Comp. Theor. Chem. 2013, 1006, 92. doi: 10.1016/j.comptc.2012.11.015
31. [31]
  (31) Torrent-Sucarrat, M.; Liu, S. B.; De Proft, F. J. Phys. Chem. A2009, 113, 3698. doi: 10.1021/jp8096583(31) Torrent-Sucarrat, M.; Liu, S. B.; De Proft, F. J. Phys. Chem. A2009, 113, 3698. doi: 10.1021/jp8096583
32. [32]
  (32) Liu, S. B. J. Chem. Sci. 2005, 117, 477; Zhong, A. G.; Rong, C.Y.; Liu, S. B. J. Phys. Chem. A 2007, 111, 3132. doi: 10.1007/BF02708352(32) Liu, S. B. J. Chem. Sci. 2005, 117, 477; Zhong, A. G.; Rong, C.Y.; Liu, S. B. J. Phys. Chem. A 2007, 111, 3132. doi: 10.1007/BF02708352
33. [33]
  (33) Valiev, M.; Bylaska, E. J.; vind, N.; Kowalski, K.; Straatsma,T. P.; Van Dam, H. J. J.; Wang, D.; Nieplocha, J.; Apra, E.;Windus, T. L.; de Jong, W. Comput. Phys. Commun. 2010, 181,1477.(33) Valiev, M.; Bylaska, E. J.; vind, N.; Kowalski, K.; Straatsma,T. P.; Van Dam, H. J. J.; Wang, D.; Nieplocha, J.; Apra, E.;Windus, T. L.; de Jong, W. Comput. Phys. Commun. 2010, 181,1477.
34. [34]
  (34) Maeda, S.; Ohno, K. J. Phys. Chem. A 2007, 111, 4527. doi: 10.1021/jp070606a(34) Maeda, S.; Ohno, K. J. Phys. Chem. A 2007, 111, 4527. doi: 10.1021/jp070606a
35. [35]
  (35) Zhao, Y.; Truhlar, D. G. Theor. Chem. Acc. 2008, 120, 215. doi: 10.1007/s00214-007-0310-x(35) Zhao, Y.; Truhlar, D. G. Theor. Chem. Acc. 2008, 120, 215. doi: 10.1007/s00214-007-0310-x
36. [36]
  (36) Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al . Gaussian 09,Revision C. 01; Gaussian, Inc.: Wallingford, CT, 2009.(36) Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al . Gaussian 09,Revision C. 01; Gaussian, Inc.: Wallingford, CT, 2009.
37. [37]
  (37) Kitaura, K.; Morokuma, K. Int. J. Quantum Chem. 1976, 10,325.
  (37) Kitaura, K.; Morokuma, K. Int. J. Quantum Chem. 1976, 10,325.

扫一扫看文章

计量

PDF下载量: 702
文章访问数: 1692
HTML全文浏览量: 115

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

水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

English

Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study

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

水团簇构象稳定性起源和本质的密度泛函理论与量子分子动力学研究

English

Towards Understanding the Origin and Nature of the Conformational Stability of Water Clusters：a Density Functional Theory and Quantum Molecular Dynamics Study

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

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs