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In this paper, we develop a Monte Carlo algorithm named the Frozen Gaussian Sampling (FGS) to solve the semiclassical Schr\"odinger equation based on the frozen Gaussian approximation. Due to the highly oscillatory structure of the wave…

Numerical Analysis · Mathematics 2021-12-21 Yantong Xie , Zhennan Zhou

In the spirit of the fewest switches surface hopping, the frozen Gaussian approximation with surface hopping (FGA-SH) method samples a path integral representation of the non-adiabatic dynamics in the semiclassical regime. An improved…

Chemical Physics · Physics 2016-10-12 Jianfeng Lu , Zhennan Zhou

In this article, we introduce the frozen Gaussian sampling (FGS) algorithm to solve the scalar wave equation in the high-frequency regime. The FGS algorithm is a Monte Carlo sampling strategy based on the frozen Gaussian approximation,…

Numerical Analysis · Mathematics 2023-09-06 Lihui Chai , Ye Feng , Zhennan Zhou

Simulating Markovian open quantum systems in the semiclassical regime poses a grand challenge for computational physics, as the highly oscillatory nature of the dynamics imposes prohibitive resolution requirements on traditional grid-based…

Quantum Physics · Physics 2025-12-17 Limin Xu , Zhen Huang , Zhennan Zhou

Quantum molecular dynamics requires an accurate representation of the molecular potential energy surface from a minimal number of electronic structure calculations, particularly for nonadiabatic dynamics where excited states are required.…

Chemical Physics · Physics 2016-08-24 Charles W. Heaps , David A. Mazziotti

We review techniques for simulating fully quantum nonadiabatic dynamics using the frozen-width moving Gaussian basis functions to represent the nuclear wavefunction. A choice of these basis functions is primarily motivated by the idea of…

Chemical Physics · Physics 2018-09-05 Loïc Joubert-Doriol , Artur F. Izmaylov

A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…

Chemical Physics · Physics 2018-04-04 Loïc Joubert-Doriol , Artur F. Izmaylov

Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…

Chemical Physics · Physics 2024-05-08 Jonathan R. Mannouch , Aaron Kelly

We develop a Floquet surface hopping (FSH) approach to deal with nonadiabatic dynamics of molecules near metal surfaces subjected to time-periodic drivings from strong light-matter interactions. The method is based on a Floquet classical…

Quantum Physics · Physics 2023-06-21 Yu Wang , Wenjie Dou

We introduce a new path integral Monte Carlo method for investigating nonadiabatic systems in thermal equilibrium and demonstrate an approach to reducing stochastic error. We derive a general path integral expression for the partition…

Chemical Physics · Physics 2019-07-11 Neil Raymond , Dmitri Iouchtchenko , Pierre-Nicholas Roy , Marcel Nooijen

Gaussian Boson Sampling (GBS) is a promising candidate for demonstrating quantum computational advantage and can be applied to solving graph-related problems. In this work, we propose Markov chain Monte Carlo-based algorithms to sample from…

Quantum Physics · Physics 2025-10-31 Yexin Zhang , Shuo Zhou , Xinzhao Wang , Ziruo Wang , Ziyi Yang , Rui Yang , Yecheng Xue , Tongyang Li

Monte Carlo simulations are a powerful tool to investigate the thermodynamic properties of atomic systems. In practice however, sampling of the complete configuration space is often hindered by high energy barriers between different regions…

Statistical Mechanics · Physics 2020-05-04 Jonas A. Finkler , Stefan Goedecker

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

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 present a Hamiltonian Monte Carlo algorithm to sample from multivariate Gaussian distributions in which the target space is constrained by linear and quadratic inequalities or products thereof. The Hamiltonian equations of motion can be…

Computation · Statistics 2013-06-06 Ari Pakman , Liam Paninski

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

We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with…

Mesoscale and Nanoscale Physics · Physics 2019-02-27 Guillermo Albareda , Aaron Kelly , Angel Rubio

We develop a surface hopping algorithm based on frozen Gaussian approximation for semiclassical matrix Schr\"odinger equations, in the spirit of Tully's fewest switches surface hopping method. The algorithm is asymptotically derived from…

Numerical Analysis · Mathematics 2017-03-30 Jianfeng Lu , Zhennan Zhou

We present a nonadiabatic classical-trajectory approach that offers the best of both worlds between fewest-switches surface hopping (FSSH) and quasiclassical mapping dynamics. This mapping approach to surface hopping (MASH) propagates the…

Chemical Physics · Physics 2023-03-29 Jonathan R. Mannouch , Jeremy O. Richardson

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
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