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条件波函数理论：分子结构与非绝热动力学的统一处理

Conditional Wave Function Theory: A Unified Treatment of Molecular Structure and Nonadiabatic Dynamics.

作者信息

Albareda Guillermo, Lively Kevin, Sato Shunsuke A, Kelly Aaron, Rubio Angel

机构信息

Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility (ETSF), Universidad del País Vasco (UPV/EHU), Av. Tolosa 72, 20018 San Sebastian, Spain.

Institute of Theoretical and Computational Chemistry, University of Barcelona, Martí i Franquès 1-11, 08028 Barcelona, Spain.

出版信息

J Chem Theory Comput. 2021 Dec 14;17(12):7321-7340. doi: 10.1021/acs.jctc.1c00772. Epub 2021 Nov 9.

DOI:10.1021/acs.jctc.1c00772
PMID:34752108
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8675140/
Abstract

We demonstrate that a conditional wave function theory enables a unified and efficient treatment of the equilibrium structure and nonadiabatic dynamics of correlated electron-ion systems. The conditional decomposition of the many-body wave function formally recasts the full interacting wave function of a closed system as a set of lower-dimensional (conditional) coupled "slices". We formulate a variational wave function ansatz based on a set of conditional wave function slices and demonstrate its accuracy by determining the structural and time-dependent response properties of the hydrogen molecule. We then extend this approach to include time-dependent conditional wave functions and address paradigmatic nonequilibrium processes including strong-field molecular ionization, laser-driven proton transfer, and nuclear quantum effects induced by a conical intersection. This work paves the road for the application of conditional wave function theory in equilibrium and out-of-equilibrium ab initio molecular simulations of finite and extended systems.

摘要

我们证明，一种条件波函数理论能够对相关电子 - 离子系统的平衡结构和非绝热动力学进行统一且高效的处理。多体波函数的条件分解将封闭系统的完整相互作用波函数形式上重铸为一组低维（条件）耦合“切片”。我们基于一组条件波函数切片制定了变分波函数假设，并通过确定氢分子的结构和与时间相关的响应特性来证明其准确性。然后，我们将此方法扩展到包含与时间相关的条件波函数，并处理典型的非平衡过程，包括强场分子电离、激光驱动的质子转移以及由锥形交叉诱导的核量子效应。这项工作为条件波函数理论在有限和扩展系统的平衡和非平衡从头算分子模拟中的应用铺平了道路。

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本文引用的文献

1
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Phys Rev Lett. 2021 Jul 2;127(1):015001. doi: 10.1103/PhysRevLett.127.015001.
2
Excited State Intramolecular Proton Transfer with Nuclear-Electronic Orbital Ehrenfest Dynamics.激发态分子内质子转移与核-电子轨道 Ehrenfest 动力学。
J Phys Chem Lett. 2021 Apr 15;12(14):3497-3502. doi: 10.1021/acs.jpclett.1c00564. Epub 2021 Apr 1.
3
Simulating Vibronic Spectra without Born-Oppenheimer Surfaces.
无需玻恩-奥本海默表面模拟电子振动光谱。
J Phys Chem Lett. 2021 Apr 1;12(12):3074-3081. doi: 10.1021/acs.jpclett.1c00073. Epub 2021 Mar 22.
4
Engineering quantum materials with chiral optical cavities.利用手性光学腔设计量子材料。
Nat Mater. 2021 Apr;20(4):438-442. doi: 10.1038/s41563-020-00801-7.
5
Signatures of a liquid-liquid transition in an ab initio deep neural network model for water.从头算深度神经网络模型中水的液-液相变特征。
Proc Natl Acad Sci U S A. 2020 Oct 20;117(42):26040-26046. doi: 10.1073/pnas.2015440117. Epub 2020 Oct 2.
6
Exciton-Phonon Interaction and Relaxation Times from First Principles.基于第一性原理的激子-声子相互作用与弛豫时间
Phys Rev Lett. 2020 Sep 4;125(10):107401. doi: 10.1103/PhysRevLett.125.107401.
7
Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite.杂化金属卤化物钙钛矿中的超快关联电荷与晶格运动
Sci Adv. 2019 May 31;5(5):eaaw5558. doi: 10.1126/sciadv.aaw5558. eCollection 2019 May.
8
Strong light-matter interactions: a new direction within chemistry.强光物质相互作用：化学的一个新方向。
Chem Soc Rev. 2019 Feb 4;48(3):937-961. doi: 10.1039/c8cs00193f.
9
A classical ride through a conical intersection.经典的锥形交叉穿越。
J Chem Phys. 2019 Jan 21;150(3):034301. doi: 10.1063/1.5080399.
10
Polariton chemistry: controlling molecular dynamics with optical cavities.极化激元化学：利用光学腔控制分子动力学
Chem Sci. 2018 Jun 12;9(30):6325-6339. doi: 10.1039/c8sc01043a. eCollection 2018 Aug 14.