Citation: SAVIN Andreas. Chemical Bonding and Interpretation of Time-Dependent Electronic Processes with Maximum Probability Domains[J]. Acta Physico-Chimica Sinica, ;2018, 34(5): 528-536. doi: 10.3866/PKU.WHXB201710111 shu

Chemical Bonding and Interpretation of Time-Dependent Electronic Processes with Maximum Probability Domains

SAVIN Andreas ^,

Laboratoire de Chimie Théorique, CNRS, and Sorbonne Université, UPMC Univ Paris 06, 4 place Jussieu, F 75252 Paris cedex 05, France

Corresponding author: SAVIN Andreas, andreas.savin@lct.jussieu.fr
Received Date: 1 September 2017
Revised Date: 25 September 2017
Accepted Date: 25 September 2017
Available Online: 11 May 2017

Tools have been designed obtain information about chemical bonds from quantum mechanical calculations. They work well for solutions of the stationary Schrödinger equation, but it is not clear whether Lewis electron pairs they aim to reproduce survive in time-dependent processes, in spite of the underlying Pauli principle being obeyed in this regime. A simple model of two same-spin non-interacting fermions in a one-dimensional box with an opaque wall, is used to study this problem, because it allows presenting the detailed structure of the wave function. It is shown that ⅰ) oscillations persisting after the Hamiltonian stopped changing produce for certain time intervals states where Lewis electron pairs are spatially separated, and ⅱ) methods (like density analysis, or the electron localization function) that are widely used for describing bonding in the stationary case, have limitations in such situations. An exception is provided by the maximum probability domain (the spatial domain that maximizes the probability to find a given number of particles in it). It is conceptually simple, and satisfactorily describes the phenomenon.
- Chemical bond,
- Time-dependent Schrödinger equation,
- Particle in a box with opaque wall
1. [1]
  Messiah, A. Quantum Mechanics; North Holland Publishing Company: Amsterdam, The Netherlands, 1967.
2. [2]
  Flügge, S. Practical Quantum Mechanics; Springer: Berlin, Germany, 1999; p. 14.
3. [3]
  Wigner, E. Phys. Rev. 1934, 46, 1002. doi: 10.1103/PhysRev.46.1002 doi: 10.1103/PhysRev.46.1002
4. [4]
  Lewis, G. N. J. Am. Chem. Soc. 1916, 38, 762. doi: 10.1021/ja02261a002 doi: 10.1021/ja02261a002
5. [5]
  Durrant, T. R.; Hodgson, M. J. P.; Ramsden, J. D.; Godby, R. W. arXiv 2015, 1505.07687.
6. [6]
  Artmann, K. Z. Naturforschg. 1946, 1, 426.
7. [7]
  Scemama, A.; Caffarel, M.; Savin, A. J. Comput. Chem. 2007, 28, 442. doi: 10.1002/jcc.20526 doi: 10.1002/jcc.20526
8. [8]
  Lüchow, A.; Petz, R. J. Comput. Chem. 2011, 32, 2619. doi: 10.1002/jcc.21841 doi: 10.1002/jcc.21841
9. [9]
  Savin, A. Reviews of Modern Quantum Chemistry: A Celebration of the Contributions of Robert G. Parr; Sen, K. D. Ed.; World Scientific: Singapore, 2002; p. 43.
10. [10]
  Bader, R. F. W. Atoms in Molecules: A Quantum Theory; Oxford University Press: Oxford, UK, 1990.
11. [11]
  Becke, A. D.; Edgecombe, K. E. J. Chem. Phys. 1990, 92, 5397. doi: 10.1063/1.458517 doi: 10.1063/1.458517
12. [12]
  Burnus, T.; Marques, M. A. L.; Gross, E. K. U. Phys. Rev. A 2005, 71, 010501. doi: 10.1103/PhysRevA.71.010501 doi: 10.1103/PhysRevA.71.010501
13. [13]
  Sini, G.; Maitre, P.; Hiberty, P. C.; Shaik, S. S. J. Mol. Struct. THEOCHEM 1991, 229, 163. doi: 10.1016/0166-1280(91)90144-9
14. [14]
  Petersilka, M.; Gross, E. Laser Physics 1999, 9, 1.
15. [15]
  Dobson, J. F. J. Chem. Phys. 1993, 98, 8870. doi: 10.1063/1.464444 doi: 10.1063/1.464444
16. [16]
  Wolfram, S. Mathematica Edition, Version 11.1; Wolfram Research, Inc.: Champaign, Illinois, USA, 2017.
1. [1]
  Rui Li , Jiayu Zhang , Anyang Li . Two Levels of Understanding of Chemical Bonds: a Case of the Bonding Model of Hypervalent Molecules. University Chemistry, 2024, 39(2): 392-398. doi: 10.3866/PKU.DXHX202308051
2. [2]
  Zixi Zou , Jingyuan Wang , Yian Sun , Qian Wang , Da-Hui Qu . Controlling molecular assembly on time scale: Time-dependent multicolor fluorescence for information encryption. Chinese Chemical Letters, 2024, 35(7): 108972-. doi: 10.1016/j.cclet.2023.108972
3. [3]
  Yang Qin , Jiangtian Li , Xuehao Zhang , Kaixuan Wan , Heao Zhang , Feiyang Huang , Limei Wang , Hongxun Wang , Longjie Li , Xianjin Xiao . Toeless and reversible DNA strand displacement based on Hoogsteen-bond triplex. Chinese Chemical Letters, 2024, 35(5): 108826-. doi: 10.1016/j.cclet.2023.108826
4. [4]
  Xueling Yu , Lixing Fu , Tong Wang , Zhixin Liu , Na Niu , Ligang Chen . Multivariate chemical analysis: From sensors to sensor arrays. Chinese Chemical Letters, 2024, 35(7): 109167-. doi: 10.1016/j.cclet.2023.109167
5. [5]
  Fangzhou Wang , Wentong Gao , Chenghui Li . A weak but inert hindered urethane bond for high-performance dynamic polyurethane polymers. Chinese Chemical Letters, 2024, 35(5): 109305-. doi: 10.1016/j.cclet.2023.109305
6. [6]
  Min Fu , Pan He , Sen Zhou , Wenqiang Liu , Bo Ma , Shiying Shang , Yaohao Li , Ruihan Wang , Zhongping Tan . An unexpected stereochemical effect of thio-substituted Asp in native chemical ligation. Chinese Chemical Letters, 2024, 35(8): 109434-. doi: 10.1016/j.cclet.2023.109434
7. [7]
  Xianxu Chu , Lu Wang , Junru Li , Hui Xu . Surface chemical microenvironment engineering of catalysts by organic molecules for boosting electrocatalytic reaction. Chinese Chemical Letters, 2024, 35(8): 109105-. doi: 10.1016/j.cclet.2023.109105
8. [8]
  Xu-Hui Yue , Xiang-Wen Zhang , Hui-Min He , Lei Qiao , Zhong-Ming Sun . Synthesis, chemical bonding and reactivity of new medium-sized polyarsenides. Chinese Chemical Letters, 2024, 35(7): 108907-. doi: 10.1016/j.cclet.2023.108907
9. [9]
  Qiongqiong Wan , Yanan Xiao , Guifang Feng , Xin Dong , Wenjing Nie , Ming Gao , Qingtao Meng , Suming Chen . Visible-light-activated aziridination reaction enables simultaneous resolving of C=C bond location and the sn-position isomers in lipids. Chinese Chemical Letters, 2024, 35(4): 108775-. doi: 10.1016/j.cclet.2023.108775
10. [10]
  Yi Luo , Lin Dong . Multicomponent remote C(sp²)-H bond addition by Ru catalysis: An efficient access to the alkylarylation of 2H-imidazoles. Chinese Chemical Letters, 2024, 35(10): 109648-. doi: 10.1016/j.cclet.2024.109648
11. [11]
  Ying Li , Long-Jie Wang , Yong-Kang Zhou , Jun Liang , Bin Xiao , Ji-Shen Zheng . An improved installation of 2-hydroxy-4-methoxybenzyl (iHmb) method for chemical protein synthesis. Chinese Chemical Letters, 2024, 35(5): 109033-. doi: 10.1016/j.cclet.2023.109033
12. [12]
  Min Huang , Ru Cheng , Shuai Wen , Liangtong Li , Jie Gao , Xiaohui Zhao , Chunmei Li , Hongyan Zou , Jian Wang . Ultrasensitive detection of microRNA-21 in human serum based on the confinement effect enhanced chemical etching of gold nanorods. Chinese Chemical Letters, 2024, 35(9): 109379-. doi: 10.1016/j.cclet.2023.109379
13. [13]
  Lian Sun , Honglei Wang , Ming Ma , Tingting Cao , Leilei Zhang , Xingui Zhou . Shape and composition evolution of Pt and Pt₃M nanocrystals under HCl chemical etching. Chinese Chemical Letters, 2024, 35(9): 109188-. doi: 10.1016/j.cclet.2023.109188
14. [14]
  Bei Li , Zhaoke Zheng . In situ monitoring of the spatial distribution of oxygen vacancies at the single-particle level. Chinese Journal of Structural Chemistry, 2024, 43(10): 100331-100331. doi: 10.1016/j.cjsc.2024.100331
15. [15]
  Yan Wang , Huixin Chen , Fuda Yu , Shanyue Wei , Jinhui Song , Qianfeng He , Yiming Xie , Miaoliang Huang , Canzhong Lu . Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries. Chinese Chemical Letters, 2024, 35(7): 109001-. doi: 10.1016/j.cclet.2023.109001
16. [16]
  Dan Luo , Jinya Tian , Jianqiao Zhou , Xiaodong Chi . Anthracene-bridged "Texas-sized" box for the simultaneous detection and uptake of tryptophan. Chinese Chemical Letters, 2024, 35(9): 109444-. doi: 10.1016/j.cclet.2023.109444
17. [17]
  Yulong Shi , Fenbei Chen , Mengyuan Wu , Xin Zhang , Runze Meng , Kun Wang , Yan Wang , Yuheng Mei , Qionglu Duan , Yinghong Li , Rongmei Gao , Yuhuan Li , Hongbin Deng , Jiandong Jiang , Yanxiang Wang , Danqing Song . Chemical construction and anti-HCoV-OC43 evaluation of novel 10,12-disubstituted aloperine derivatives as dual cofactor inhibitors of TMPRSS2 and SR-B1. Chinese Chemical Letters, 2024, 35(5): 108792-. doi: 10.1016/j.cclet.2023.108792
18. [18]
  Guangchang Yang , Shenglong Yang , Jinlian Yu , Yishun Xie , Chunlei Tan , Feiyan Lai , Qianqian Jin , Hongqiang Wang , Xiaohui Zhang . Regulating local chemical environment in O3-type layered sodium oxides by dual-site Mg²⁺/B³⁺ substitution achieves durable and high-rate cathode. Chinese Chemical Letters, 2024, 35(9): 109722-. doi: 10.1016/j.cclet.2024.109722
19. [19]
  Wangyan Hu , Ke Li , Xiangnan Dou , Ning Li , Xiayan Wang . Nano-sized stationary phase packings retained by single-particle frit for microchip liquid chromatography. Chinese Chemical Letters, 2024, 35(4): 108806-. doi: 10.1016/j.cclet.2023.108806
20. [20]
  Wenling Yuan , Fengli Li , Zhe Chen , Qiaoxin Xu , Zhenhua Guan , Nanyu Yao , Zhengxi Hu , Junjun Liu , Yuan Zhou , Ying Ye , Yonghui Zhang . AbnI: An α-ketoglutarate-dependent dioxygenase involved in brassicicene CH functionalization and ring system rearrangement. Chinese Chemical Letters, 2024, 35(5): 108788-. doi: 10.1016/j.cclet.2023.108788

Get Citation

PDF

XML

Metrics

PDF Downloads(8)
Abstract views(412)
HTML views(15)

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