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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

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

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

We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…

Computational Physics · Physics 2018-11-21 Jerome Daligault , Dmitry Mozyrsky

Recently proposed non-adiabatic ring polymer molecular dynamics (NRPMD) approach has shown to provide accurate quantum dynamics by incorporating explicit electronic state descriptions and nuclear quantizations. Here, we present a rigorous…

Chemical Physics · Physics 2019-07-24 Sutirtha N. Chowdhury , Pengfei Huo

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

We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…

Chemical Physics · Physics 2012-06-28 Tomas Zimmermann , Jiri Vanicek

A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…

Chemical Physics · Physics 2020-11-06 Sudip Sasmal , Oriol Vendrell

We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…

Chemical Physics · Physics 2024-04-23 Richard Einsele , Roland Mitrić

Accurate and efficient simulation of nonadiabatic dynamics is highly desirable for understanding charge and energy transfer in complex systems. A key criterion for obtaining an accurate method is conservation of the Quantum Boltzmann…

Chemical Physics · Physics 2025-10-07 Lauren E. Cook , Timothy J. H. Hele

We develop a scheme of fast forward of adiabatic spin dynamics of quantum entangled states. We settle the quasi-adiabatic dynamics by adding the regularization terms to the original Hamiltonian and then accelerate it with use of a large…

Quantum Physics · Physics 2018-05-25 Iwan Setiawan , Bobby Eka Gunara , Shumpei Masuda , Katsuhiro Nakamura

We extend the Mixed Quantum-Classical Initial Value Representation (MQC-IVR), a semiclassical method for computing real-time correlation functions, to electronically nonadiabatic systems using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian…

Chemical Physics · Physics 2018-01-17 Matthew S. Church , Timothy J. H. Hele , Gregory S. Ezra , Nandini Ananth

The treatment of time-dependent dynamics of quantum systems involving multiple states poses considerable technical challenges. One of the most efficient approaches in treating such systems is the Morris-Shore (MS) transformation which…

Quantum Physics · Physics 2022-09-28 K. N. Zlatanov , A. A. Rangelov , N. V. Vitanov

An approach to non-adiabatic dynamics of atoms in molecular and condensed matter systems under general non-equilibrium conditions is proposed. In this method interaction between nuclei and electrons is considered explicitly up to the second…

Materials Science · Physics 2018-08-01 L. Kantorovich

We build on the concept of eigenvector continuation to develop an efficient multi-state method for the rigorous and smooth interpolation of a small training set of many-body wavefunctions through chemical space at mean-field cost. The…

Chemical Physics · Physics 2024-05-02 Kemal Atalar , Yannic Rath , Rachel Crespo-Otero , George H. Booth

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

Direct simulation of the von Neumann dynamics for a general (pure or mixed) quantum state can often be expensive. One prominent example is the real-time time-dependent density functional theory (rt-TDDFT), a widely used framework for the…

Numerical Analysis · Mathematics 2022-10-19 Dong An , Di Fang , Lin Lin

A generalized formalism of the so-called non-adiabatic quantum molecular dynamics is presented, which applies for atomic many-body systems in external laser fields. The theory treats the nuclear dynamics and electronic transitions…

Atomic Physics · Physics 2007-05-23 Thomas Kunert , Ruediger Schmidt

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

Excited-state molecular dynamics (ESMD) simulations near conical intersections (CIs) pose significant challenges when using machine learning potentials (MLPs). Although MLPs have gained recognition for their integration into mixed…

Chemical Physics · Physics 2025-01-17 Sung Wook Moon , Soohaeng Yoo Willow , Tae Hyeon Park , Seung Kyu Min , Chang Woo Myung
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