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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

Rare nonadiabatic reactions are a key component of many important molecular processes but are challenging to capture with direct dynamical simulations. In this paper, we combine our recently developed mapping approach to surface hopping…

Chemical Physics · Physics 2026-03-19 Danial Ghamari , Jeremy O. Richardson

In the paper we derive a semiclassical model for surface hopping allowing quantum dynamical non-adiabatic transition between different potential energy surfaces in which cases the classical Born-Oppenheimer approximation breaks down. The…

Numerical Analysis · Mathematics 2014-05-06 Lihui Chai , Shi Jin , Qin Li , Omar Morandi

This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum…

Computational Physics · Physics 2019-08-15 Wanghuai Zhou , Arkajit Mandal , Pengfei Huo

Exact and nonperturbative quantum master equation can be constructed via the calculus on path integral. It results in hierarchical equations of motion for the reduced density operator. Involved are also a set of well--defined auxiliary…

Statistical Mechanics · Physics 2015-05-13 Jian Xu , Rui-Xue Xu , YiJing Yan

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

A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…

Mesoscale and Nanoscale Physics · Physics 2024-05-06 Samuel L. Rudge , Christoph Kaspar , Robin L. Grether , Steffen Wolf , Gerhard Stock , Michael Thoss

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

We propose a nonperturbative quantum dissipation theory, in term of hierarchical quantum master equation. It may be used with a great degree of confidence to various dynamics systems in condensed phases. The theoretical development is…

Statistical Mechanics · Physics 2015-05-14 Rui-Xue Xu , Bao-Ling Tian , Jian Xu , Qiang Shi , YiJing Yan

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 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 introduce an approach for quantum computing in continuous time based on the Lewis-Riesenfeld dynamic invariants. This approach allows, under certain conditions, for the design of quantum algorithms running on a nonadiabatic regime. We…

Quantum Physics · Physics 2011-08-18 M. S. Sarandy , E. I. Duzzioni , R. M. Serra

A class of surface hopping algorithms is studied comparing two recent Landau-Zener (LZ) formulas for the probability of nonadiabatic transitions. One of the formulas requires a diabatic representation of the potential matrix while the other…

Chemical Physics · Physics 2015-06-19 Andrey K. Belyaev , Caroline Lasser , Giulio Trigila

We propose a method to produce fast transitionless dynamics for finite-dimensional quantum systems without requiring additional Hamiltonian components not included in the initial control setup, remaining close to the true adiabatic path at…

Quantum Physics · Physics 2018-11-09 Francesco Petiziol , Benjamin Dive , Florian Mintert , Sandro Wimberger

We introduce an alternative way to derive the generalized form of the master equation recently presented by J. P. Pekola et al. [Phys. Rev. Lett. 105, 030401 (2010)] for an adiabatically steered two-level quantum system interacting with a…

Quantum Physics · Physics 2011-12-22 J. Salmilehto , P. Solinas , J. Ankerhold , M. Möttönen

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

The Landau--Zener (LZ) type classical-trajectory surface-hopping algorithm is applied to the nonadiabatic nuclear dynamics of the ammonia cation after photoionization of the ground-state neutral molecule to the excited states of the cation.…

Chemical Physics · Physics 2015-06-23 Andrey K. Belyaev , Wolfgang Domcke , Caroline Lasser , Giulio Trigila

An extension of the CCS-method [Chem. Phys. 2004, 304, p. 103-120] for simulating non-adiabatic dynamics with quantum effects of the nuclei is put forward. The time-dependent Schr\"{o}dinger equation for the motion of the nuclei is solved…

Chemical Physics · Physics 2016-07-27 Alexander Humeniuk , Roland Mitrić

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

The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…

Quantum Physics · Physics 2021-01-06 Pauline J. Ollitrault , Guglielmo Mazzola , Ivano Tavernelli