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We perform extensive benchmark comparisons of surface hopping dynamics with numerically exact calculations for the spin-boson model over a wide range of energetic and coupling parameters as well as temperature. We find that deviations from…

Mesoscale and Nanoscale Physics · Physics 2016-04-04 Hsing-Ta Chen , David R. Reichman

This study introduces the FSSH-2 scheme, a redefined and numerically stable adiabatic Fewest Switches Surface Hopping (FSSH) method for mixed quantum-classical dynamics. It reformulates the standard FSSH hopping probability without…

Computational Physics · Physics 2024-01-19 Leonardo Araujo , Caroline Lasser , Burkhard Schmidt

Coarse-grained (CG) conformational surface hopping (SH) adapts the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to accurately describe classical molecular dynamics at a…

Soft Condensed Matter · Physics 2021-02-03 Joseph F. Rudzinski , Tristan Bereau

A new scheme is proposed for modeling molecular nonadiabatic dynamics near metal surfaces. The charge-transfer character of such dynamics is exploited to construct an efficient reduced representation for the electronic structure. In this…

Chemical Physics · Physics 2020-09-24 Zuxin Jin , Joseph E. Subotnik

Mouse-tracking recording techniques are becoming very attractive in experimental psychology. They provide an effective means of enhancing the measurement of some real-time cognitive processes involved in categorization, decision-making, and…

Applications · Statistics 2019-12-18 Antonio Calcagnì , Luigi Lombardi , Marco D'Alessandro

We propose a general framework for a hybrid continuous-discrete algorithm that integrates continuous-time deterministic dynamics with Metropolis-Hastings steps to combine search dynamics with and without detailed balance. Our purpose is to…

Statistical Mechanics · Physics 2024-10-31 Timothée Leleu , Samuel Reifenstein

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

A general theoretical framework is derived for the recently developed multi-state trajectory (MST) approach from the time dependent Schr\"odinger equation, resulting in equations of motion for coupled nuclear-electronic dynamics equivalent…

Chemical Physics · Physics 2017-09-13 Guohua Tao

We present a novel shape-approximating anisotropic re-meshing algorithm as a geometric generalization of the adaptive moving mesh method. Conventional moving mesh methods reduce the interpolation error of a mesh that discretizes a given…

Computational Geometry · Computer Science 2023-06-21 Nicolas Nebel , Albert Chern

We implement a rare-event sampling scheme for quantifying the rate of thermally-activated nonadiabatic transitions in the condensed phase. Our QM/MM methodology uses the recently developed INAQS package to interface between an elementary…

Chemical Physics · Physics 2023-03-23 Alec J. Coffman , Zuxin Jin , Junhan Chen , Joseph E. Subotnik , D. Vale Cofer-Shabica

Non-equilibrium Markov State Modeling (MSM) has recently been proposed [Phys. Rev. E 94, 053001 (2016)] as a possible route to construct a physical theory of sliding friction from a long steady state atomistic simulation: the approach…

Statistical Mechanics · Physics 2017-10-17 M. Teruzzi , F. Pellegrini , A. Laio , E. Tosatti

The quantum-classical Liouville equation offers a rigorous approach to nonadiabatic quantum dynamics based on surface hopping type trajectories. However, in practice the applicability of this approach has been limited to short times owing…

Chemical Physics · Physics 2015-06-16 Aaron Kelly , Thomas E. Markland

In this work, a novel ring polymer representation for multi-level quantum system is proposed for thermal average calculations. The proposed presentation keeps the discreteness of the electronic states: besides position and momentum, each…

Chemical Physics · Physics 2017-05-24 Jianfeng Lu , Zhennan Zhou

While surface-hopping has emerged as a powerful method to simulate non-adiabatic dynamics in large molecules, the ad hoc nature of the necessary velocity adjustments and decoherence corrections in the algorithm somewhat reduces its…

Chemical Physics · Physics 2024-01-17 Lucien Dupuy , Anton Rikus , Neepa T. Maitra

Surface hopping algorithms are popular tools to study dynamics of the quantum-classical mixed systems. In this paper, we propose a surface hopping algorithm in diabatic representations, based on time dependent perturbation theory and…

Numerical Analysis · Mathematics 2022-10-19 Di Fang , Jianfeng Lu

We propose a surface hopping Gaussian beam method to numerically solve a class of high frequency linear transport systems in high spatial dimensions, based on asymptotic analysis. The stochastic surface hopping is combined with Gaussian…

Numerical Analysis · Mathematics 2017-03-24 Zhenning Cai , Jianfeng Lu

Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…

Chemical Physics · Physics 2016-05-24 Alexander White , Sergei Tretiak , Dmitry Mozyrsky

We investigate a simple and robust scheme for choosing the phases of adiabatic electronic states smoothly (as a function of geometry) so as to maximize the performance of ab initio non-adiabatic dynamics methods. Our approach is based upon…

Chemical Physics · Physics 2019-09-26 Zeyu Zhou , Zuxin Jin , Tian Qiu , Andrew M. Rappe , Joseph Eli Subotnik

There exist several methods for simulating biological and physical systems as represented by chemical reaction networks. Systems with low numbers of particles are frequently modelled as discrete-state Markov jump processes and are typically…

Quantitative Methods · Quantitative Biology 2022-10-24 Joshua C. Kynaston , Christian A Yates , Anna Hekkink , Chris Guiver

We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…

Chemical Physics · Physics 2020-03-03 Johan E. Runeson , Jeremy O. Richardson