A Phase-Space Electronic Hamiltonian For Vibrational Circular Dichroism,Journal of Chemical Theory and Computation

当前位置： X-MOL 学术 › J. Chem. Theory Comput. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

A Phase-Space Electronic Hamiltonian For Vibrational Circular Dichroism
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2024-09-03 , DOI: 10.1021/acs.jctc.4c00662
Titouan Duston ₁ , Zhen Tao ₁ , Xuezhi Bian ₁ , Mansi Bhati ₁ , Jonathan Rawlinson ₂ , Robert G Littlejohn ₃ , Zheng Pei ₄ , Yihan Shao ₄ , Joseph E Subotnik ₁

Affiliation

We show empirically that a phase-space non-Born–Oppenheimer electronic Hamiltonian approach to quantum chemistry (where the electronic Hamiltonian is parametrized by both nuclear position and momentum, Ĥ_PS(R,P)) is both a practical and accurate means to recover vibrational circular dichroism spectra. We further hypothesize that such a phase-space approach may lead to very new dynamical physics beyond spectroscopic circular dichroism, with potential implications for understanding chiral induced spin selectivity (CISS), noting that classical phase-space approaches conserve the total nuclear plus electronic momentum, whereas classical Born–Oppenheimer approaches do not (they conserve only the nuclear momentum).

中文翻译：

振动圆二色性的相空间电子哈密顿量

我们凭经验证明，量子化学的相空间非玻恩-奥本海默电子哈密顿量方法（其中电子哈密顿量通过核位置和动量进行参数化， Ĥ _PS ( R , P ) ）是一种实用且准确的方法来恢复振动圆二色光谱。我们进一步假设这种相空间方法可能会导致超越光谱圆二色性的非常新的动力学物理学，对理解手性诱导自旋选择性（CISS）具有潜在影响，并指出经典的相空间方法守恒总核加电子动量，而经典的玻恩-奥本海默方法则不然（它们只守恒核动量）。

更新日期：2024-09-03

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南