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We present a first principles molecular dynamics approach that is based on time-reversible ex- tended Lagrangian Born-Oppenheimer molecular dynamics [Phys. Rev. Lett. 100, 123004 (2008)] in the limit of vanishing self-consistent field…

Chemical Physics · Physics 2015-06-18 Petros Souvatzis , Anders M. N. Niklasson

We present a new formulation of ab initio molecular dynamics which exploits the efficiency of plane waves in adaptive curvilinear coordinates, and thus provides an accurate treatment of first-row elements. The method is used to perform a…

mtrl-th · Physics 2009-10-28 Francois Gygi

The Mixed Quantum-Classical Initial Value Representation (MQC-IVR) is a recently introduced approximate semiclassical (SC) method for the calculation of real-time quantum correlation functions. MQC-IVR employs a modified Filinov filtration…

Chemical Physics · Physics 2017-09-25 Matthew S. Church , Sergey V. Antipov , Nandini Ananth

Quantum trajectories, originating from the de Broglie-Bohm (dBB) hydrodynamic description of quantum mechanics, are used to construct time-correlation functions in an initial value representation (IVR). The formulation is fully quantum…

Quantum Physics · Physics 2009-11-10 Eric R. Bittner

We present a novel approach to calculate molecular IR spectra based on semiclassical molecular dynamics. The main advance from a previous semiclassical method [M. Micciarelli, R. Conte, J. Suarez, M. Ceotto J. Chem. Phys. 149, 064115…

Chemical Physics · Physics 2019-05-15 Marco Micciarelli , Fabio Gabas , Riccardo Conte , Michele Ceotto

We demonstrate that the quantum dynamics of a many-body Fermi-Bose system can be simulated using a Gaussian phase-space representation method. In particular, we consider the application of the mixed fermion-boson model to ultracold quantum…

Quantum Gases · Physics 2015-03-13 M. Ogren , K. V. Kheruntsyan , J. F. Corney

We describe a new approach based on semiclassical molecular dynamics that allows to simulate infrared absorption or emission spectra of molecular systems with inclusion of anharmonic intensities. This is achieved from semiclassical power…

Chemical Physics · Physics 2018-11-12 Marco Micciarelli , Riccardo Conte , Jaime Suarez , Michele Ceotto

The recently introduced mixed time-averaging semiclassical initial value representation molecular dynamics method for spectroscopic calculations [M. Buchholz, F. Grossmann, and M. Ceotto, J. Chem. Phys. 144, 094102 (2016)] is applied to…

Quantum Physics · Physics 2017-11-22 Max Buchholz , Frank Grossmann , Michele Ceotto

This article shows a proof of concept regarding the feasibility of ab initio molecular simulation, wherein the wavefunctions and the positions of nuclei are simultaneously determined by the quantum algorithm, as is realized by the so-called…

Quantum Physics · Physics 2025-04-23 Ichio Kikuchi , Akihito Kikuchi

A mixed semiclassical initial value representation expression for spectroscopic calculations is derived. The formulation takes advantage of the time-averaging filtering and the hierarchical properties of different trajectory based…

Quantum Physics · Physics 2016-05-27 Max Buchholz , Frank Grossmann , Michele Ceotto

We present and test an approximate method for the semiclassical calculation of vibrational spectra. The approach is based on the mixed time-averaging semiclassical initial value representation method, which is simplified to a form that…

Chemical Physics · Physics 2018-03-22 Max Buchholz , Frank Grossmann , Michele Ceotto

We report a computationally tractable approach to first principles investigation of time-dependent current of molecular devices under a step-like pulse. For molecular devices, all the resonant states below Fermi level contribute to the…

Mesoscale and Nanoscale Physics · Physics 2015-05-20 Yanxia Xing , Bin Wang , Jian Wang

First-principles molecular dynamics simulation based on a plane wave/pseudopotential implementation of density functional theory is adopted to investigate atomic scale energy transport for semiconductors (silicon and germanium). By imposing…

Computational Physics · Physics 2016-02-02 Pengfei Ji , Yuwen Zhang

To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…

Numerical Analysis · Mathematics 2026-02-27 Siu Wun Cheung , Youngsoo Choi , Jean-Luc Fattebert , Jonas Kaufman , Daniel Osei-Kuffuor

Egorov's theorem on the classical propagation of quantum observables is related to prominent quasi-classical descriptions of quantum molecuar dynamics as the linearized semiclassical initial value representation (LSC-IVR), the Wigner phase…

Chemical Physics · Physics 2014-10-24 Johannes Keller , Caroline Lasser

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

This article is an introduction to a new approach to first principles electronic structure calculation. The starting point is the Hartree-Fock-Roothaan equation, in which molecular integrals are approximated by polynomials by way of Taylor…

Computational Physics · Physics 2019-07-18 Akihito Kikuchi

The semiclassical Double Herman-Kluk Initial Value Representation is an accurate approach to computing quantum real time correlation functions, but its applications are limited by the need to evaluate an oscillatory integral. In previous…

Chemical Physics · Physics 2019-10-23 Matthew S. Church , Nandini Ananth

We simulate the nonadiabatic dynamics of photo-induced isomerization and dissociation in ethylene using ab initio classical trajectories in an extended phase space of nuclear and electronic variables. This is achieved by employing the…

Chemical Physics · Physics 2023-08-04 Ken Miyazaki , Nandini Ananth

We show that a single change in the derivation of the linearized semiclassical-initial value representation (LSC-IVR or classical Wigner approximation) results in a classical dynamics which conserves the quantum Boltzmann distribution. We…

Chemical Physics · Physics 2015-04-10 Timothy J. H. Hele , Michael J. Willatt , Andrea Muolo , Stuart C. Althorpe
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