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Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…

Chemical Physics · Physics 2014-08-08 Wei Feng , Luting Xu , Xin-Qi Li , Weihai Fang , YiJing Yan

Trajectory-based mixed quantum-classical approaches to coupled electron-nuclear dynamics suffer from well-studied problems such as the lack of (or incorrect account for) decoherence in the trajectory surface hopping method and the inability…

Quantum Physics · Physics 2016-02-29 Federica Agostini , Seung Kyu Min , Ali Abedi , E. K. U. Gross

We present a novel quantum-classical approach to non-adiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the…

Chemical Physics · Physics 2015-08-19 Seung Kyu Min , Federica Agostini , E. K. U. Gross

We describe a path-integral approach for including nuclear quantum effects in non-adiabatic chemical dynamics simulations. For a general physical system with multiple electronic energy levels, a corresponding isomorphic Hamiltonian is…

Statistical Mechanics · Physics 2018-06-05 Xuecheng Tao , Philip Shushkov , Thomas Miller

While the treatment of conical intersections in molecular dynamics generally requires nonadiabatic approaches, the Born-Oppenheimer adiabatic approximation is still adopted as a valid alternative in certain circumstances. In the context of…

Chemical Physics · Physics 2020-09-16 Jonathan I. Rawlinson , Cesare Tronci

Nonadiabatic dynamical processes are one of the most important quantum mechanical phenomena in chemical, materials, biological, and environmental molecular systems, where the coupling between different electronic states is either inherent…

Chemical Physics · Physics 2022-05-24 Jian Liu , Xin He , Baihua Wu

We present a method to study rare nonadiabatic dynamics in open quantum systems using transition path sampling and quantum jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely…

Statistical Mechanics · Physics 2021-12-08 Addison J. Schile , David T. Limmer

We present a means of studying rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. This approach allows for elucidation of reactive paths for dissipative, nonadiabatic…

Chemical Physics · Physics 2022-11-09 Michelle C. Anderson , Addison J. Schile , David T. Limmer

An approach to the quantum-classical mechanics of phase space dependent operators, which has been proposed recently, is remodeled as a formalism for wave fields. Such wave fields obey a system of coupled non-linear equations that can be…

Quantum Physics · Physics 2007-05-23 Alessandro Sergi

This report presents a new approach for treating the coupling of electrons and nuclei in quantum mechanical calculations for molecules and condensed matter. It includes the standard "Born-Oppenheimer approximation" as a special case but…

Chemical Physics · Physics 2013-06-28 Gerald I. Kerley

Quantum systems are typically subject to various environmental noise sources. Treating these environmental disturbances with a system-bath approach beyond weak coupling one must refer to numerical methods as, for example, the numerically…

Quantum Physics · Physics 2021-12-08 Timo Palm , Peter Nalbach

Adequate simulation of non-adiabatic dynamics through conical intersection requires account for a non-trivial geometric phase (GP) emerging in electronic and nuclear wave-functions in the adiabatic representation. Popular mixed…

Chemical Physics · Physics 2015-07-20 Rami Gherib , Ilya G. Ryabinkin , Artur F. Izmaylov

Path integral Monte Carlo approach is used to study the coupled quantum dynamics of the electron and nuclei in hydrogen molecule ion. The coupling effects are demonstrated by comparing differences in adiabatic Born--Oppenheimer and…

Chemical Physics · Physics 2008-12-29 I. Kylänpää , M. Leino , T. T. Rantala

We consider nonadiabatic systems in which the classical Born-Oppenheimer approximation breaks down. We present a general theory that accurately captures the full transmitted wavepacket after multiple transitions through either a single or…

Chemical Physics · Physics 2018-04-16 Benjamin D. Goddard , Tim Hurst

Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…

Chemical Physics · Physics 2022-07-20 Yanze Wu , Xuezhi Bian , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat…

Chemical Physics · Physics 2024-08-20 Jonathan R. Mannouch , Aaron Kelly

Nonadiabatic transition dynamics lies at the core of many electron/hole transfer, photoactivated, and vacuum field-coupled processes. About a century after Ehrenfest proposed "Phasenraum" and the Ehrenfest theorem, we report a conceptually…

Quantum Physics · Physics 2024-04-09 Baihua Wu , Xin He , Jian Liu

Every physical regime is some sort of approximation of reality. One lesser-known realm that is the semiquantal regime, which may be used to describe systems with both classical and quantum subcomponents. In the present review, we discuss…

Chaotic Dynamics · Physics 2009-11-07 Mason A. Porter

Nonadiabatic geometric phases are only dependent on the evolution path of a quantum system but independent of the evolution details, and therefore quantum computation based on nonadiabatic geometric phases is robust against control errors.…

Quantum Physics · Physics 2020-06-09 K. Z. Li , P. Z. Zhao , D. M. Tong

We consider non-adiabatic transitions in multiple dimensions, which occur when the Born-Oppenheimer approximation breaks down. We present a general, multi-dimensional algorithm which can be used to accurately and efficiently compute the…

Chemical Physics · Physics 2018-04-16 V. Betz , B. D. Goddard , T. Hurst
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