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We demonstrate that, for systems with spin-orbit coupling and an odd number of electrons, the standard fewest switches surface hopping (FSSH) algorithm does not conserve the total linear or angular momentum. This lack of conservation arises…

Chemical Physics · Physics 2023-11-29 Yanze Wu , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

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 surface-hopping algorithm recently derived from the exact factorization approach, SHXF, [Ha, Lee, Min, J. Phys. Chem. Lett. 9, 1097 (2018)] introduces an additional term in the electronic equation of surface-hopping, which couples…

Chemical Physics · Physics 2022-02-08 Patricia Vindel-Zandbergen , Spiridoula Matsika , Neepa T. Maitra

We present a novel semiclassical phase-space surface hopping approach that goes beyond the Born-Oppenheimer approximation and all existing surface hopping formalisms. We demonstrate that working with a correct phase-space electronic…

Chemical Physics · Physics 2024-10-03 Xuezhi Bian , Yanze Wu , Tian Qiu , Tao Zhen , Joseph E. Subotnik

A theoretical justification of the empirical surface hopping method for the laser-driven molecular dynamics is given utilizing the formalism of the exact factorization of the molecular wavefunction [Abedi et al., PRL $\textbf{105}$, 123002…

Chemical Physics · Physics 2017-07-05 T. Fiedlschuster , J. Handt , E. K. U. Gross , R. Schmidt

We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…

Chemical Physics · Physics 2020-09-07 Eugene Stolyarov , Alexander White , Dmitry Mozyrsky

Surface hopping algorithms, as an important class of quantum dynamics simulation algorithms for non-adiabatic dynamics, are typically performed in the adiabatic representation, which can break down in the presence of ill-defined adiabatic…

Numerical Analysis · Mathematics 2022-05-06 Zhenning Cai , Di Fang , Jianfeng Lu

The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…

Chemical Physics · Physics 2013-12-16 Wei Feng , Luting Xu , Xin-Qi Li , Weihai Fang

Quantum kinetically constrained models can exhibit a wealth of dynamical phenomena ranging from anomalous transport to Hilbert-space fragmentation (HSF). We study a class of one-dimensional particle number conserving systems where particle…

Statistical Mechanics · Physics 2023-11-02 Cheng Wang , Zhi-Cheng Yang

Trajectory surface hopping (TSH) is one of the most widely used quantum-classical algorithms for nonadiabatic molecular dynamics. Despite its empirical effectiveness and popularity, a rigorous derivation of TSH as the classical limit of a…

Chemical Physics · Physics 2013-01-11 J. M. Escartín , P. Romaniello , L. Stella , P. -G. Reinhard , E. Suraud

We analyze a quantum-classical hybrid system of steadily precessing slow classical localized magnetic moments, forming a head-to-head domain wall, embedded into an open quantum system of fast nonequilibrium electrons. The electrons reside…

Mesoscale and Nanoscale Physics · Physics 2020-10-29 Utkarsh Bajpai , Branislav K. Nikolic

Independent electron surface hopping (IESH) is a computational algorithm for simulating the mixed quantum-classical molecular dynamics of adsorbate atoms and molecules interacting with metal surfaces. It is capable of modelling the…

Chemical Physics · Physics 2023-02-22 James Gardner , Daniel Corken , Svenja M. Janke , Scott Habershon , Reinhard J. Maurer

Fewest-switches surface hopping is studied in the context of quantum-classical Liouville dynamics. Both approaches are mixed quantum-classical theories that provide a way to describe and simulate the nonadiabatic quantum dynamics of…

Quantum Physics · Physics 2016-05-27 Raymond Kapral

Smoothed particle hydrodynamics (SPH) is positioned as having ideal conservation properties. When properly implemented, conservation of total mass, energy, and both linear and angular momentum is guaranteed exactly, up to machine precision.…

Instrumentation and Methods for Astrophysics · Physics 2021-07-16 Oleg Korobkin , Hyun Lim , Irina Sagert , Julien Loiseau , Christopher Mauney , M. Alexander R. Kaltenborn , Bing-Jyun Tsao , Wesley P. Even

Nuclear Berry curvature effects emerge from electronic spin degeneracy and canlead to non-trivial spin-dependent (nonadiabatic) nuclear dynamics. However, such effects are completely neglected in all current mixed quantum-classical methods…

Chemical Physics · Physics 2022-08-29 Xuezhi Bian , Yanze Wu , Jonathan Rawlinson , Robert G. Littlejohn , Joseph E. Subotnik

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

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

A symmetry preserving framework for the study of continuum Quantum Chromodynamics (QCD) is obtained from a truncated solution of the QCD equations of motion or QCD's Dyson-Schwinger equations (DSEs). A nonperturbative solution of the DSEs…

Nuclear Theory · Physics 2016-04-20 Jorge Segovia

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
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