Simulating Magnetic Field-Driven Real-Time Quantum Dynamics Using London Nuclear-Electronic Orbital Approach.

IF 5.7 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2025-04-18 DOI:10.1021/acs.jctc.5c00273

Diandong Tang,Aodong Liu,Tanner Culpitt,Sharon Hammes-Schiffer,Xiaosong Li

{"title":"Simulating Magnetic Field-Driven Real-Time Quantum Dynamics Using London Nuclear-Electronic Orbital Approach.","authors":"Diandong Tang,Aodong Liu,Tanner Culpitt,Sharon Hammes-Schiffer,Xiaosong Li","doi":"10.1021/acs.jctc.5c00273","DOIUrl":null,"url":null,"abstract":"Harnessing a static magnetic field to drive molecular vibrations presents a promising avenue for controlling chemical processes. However, the coupling of nuclear dynamics with an external magnetic field has largely been explored only through classical approximations. In this work, we introduce a time-dependent quantum dynamics formalism based on London nuclear-electronic orbitals, enabling the simulation of magnetic field-driven quantum dynamics. Through simulations of HCN and H2CO molecules, we provide a detailed analysis of how the relative orientation of the magnetic field and vibrational symmetry influence the resulting quantum dynamics. Our findings reveal field-induced mode couplings and symmetry-dependent effects, offering new insights into the role of magnetic fields in vibrational control. This work establishes a quantum mechanical framework for understanding and manipulating vibrational dynamics using external magnetic fields, paving the way for novel applications in spectroscopy, reaction dynamics, and quantum control.","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":"5 1","pages":""},"PeriodicalIF":5.7000,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.5c00273","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

Harnessing a static magnetic field to drive molecular vibrations presents a promising avenue for controlling chemical processes. However, the coupling of nuclear dynamics with an external magnetic field has largely been explored only through classical approximations. In this work, we introduce a time-dependent quantum dynamics formalism based on London nuclear-electronic orbitals, enabling the simulation of magnetic field-driven quantum dynamics. Through simulations of HCN and H2CO molecules, we provide a detailed analysis of how the relative orientation of the magnetic field and vibrational symmetry influence the resulting quantum dynamics. Our findings reveal field-induced mode couplings and symmetry-dependent effects, offering new insights into the role of magnetic fields in vibrational control. This work establishes a quantum mechanical framework for understanding and manipulating vibrational dynamics using external magnetic fields, paving the way for novel applications in spectroscopy, reaction dynamics, and quantum control.

查看原文本刊更多论文

利用伦敦核电子轨道方法模拟磁场驱动的实时量子动力学。

利用静态磁场驱动分子振动为控制化学过程提供了一条前景广阔的途径。然而，核动力学与外部磁场的耦合在很大程度上只能通过经典近似来探索。在这项工作中，我们引入了基于伦敦核电子轨道的随时间变化的量子动力学形式，从而能够模拟磁场驱动的量子动力学。通过模拟 HCN 和 H2CO 分子，我们详细分析了磁场的相对方向和振动对称性如何影响所产生的量子动力学。我们的研究结果揭示了磁场诱导的模式耦合和对称性效应，为了解磁场在振动控制中的作用提供了新的视角。这项研究为利用外部磁场理解和操纵振动动力学建立了量子力学框架，为光谱学、反应动力学和量子控制领域的新型应用铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Chemical Theory and Computation 化学-物理：原子、分子和化学物理

CiteScore

9.90

自引率

16.40%

发文量

568

审稿时长

1 months

期刊介绍： The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.