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We present a time-reversible Born-Oppenheimer molecular dynamics scheme, based on self-consistent Hartree-Fock or density functional theory, where both the nuclear and the electronic degrees of freedom are propagated in time. We show how a…

Materials Science · Physics 2009-11-11 Anders M. N. Niklasson , C. J. Tymczak , Matt Challacombe

Born-Oppenheimer dynamics is shown to provide an accurate approximation of time-independent Schr\"odinger observables for a molecular system with an electron spectral gap, in the limit of large ratio of nuclei and electron masses, without…

Mathematical Physics · Physics 2011-09-21 Christian Bayer , Håkon Hoel , Petr Plecháč , Anders Szepessy , Raúl Tempone

We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Chemical Physics · Physics 2025-11-14 Chen Li , Ryan Requist , E. K. U. Gross

Born-Oppenheimer Molecular Dynamics (BOMD) is a powerful but expensive technique. The main bottleneck in a density functional theory bomd calculation is the solution to the Kohn-Sham (KS) equations, that requires an iterative procedure that…

Chemical Physics · Physics 2021-09-23 Etienne Polack , Geneviève Dusson , Benjamin Stamm , Filippo Lipparini

We present a new method which combines Car-Parrinello and Born-Oppenheimer molecular dynamics in order to accelerate density functional theory based ab-initio simulations. Depending on the system a gain in efficiency of one to two orders of…

Materials Science · Physics 2007-05-23 Thomas D. Kühne , Matthias Krack , Fawzi R. Mohamed , Michele Parrinello

This article proposes a so-called Quasi Time-Reversible (QTR G-Ext) scheme based on Grassmann extrapolation of density matrices for an accurate calculation of initial guesses in Born-Oppenheimer Molecular Dynamics simulations. The method…

Extended Lagrangian Born-Oppenheimer molecular dynamics [Phys. Rev. Lett., ${\bf 100}$, 123004 (2008)] is formulated for general Hohenberg-Kohn density functional theory and compared to the extended Lagrangian framework of first principles…

Materials Science · Physics 2017-09-13 Anders M. N. Niklasson

We present the construction of an exponentially accurate time-dependent Born-Oppenheimer approximation for molecular quantum mechanics. We study molecular systems whose electron masses are held fixed and whose nuclear masses are…

Mathematical Physics · Physics 2009-10-31 George A. Hagedorn , Alain Joye

We obtain thermostatted ring polymer molecular dynamics (TRPMD) from exact quantum dynamics via Matsubara dynamics, a recently-derived form of linearization which conserves the quantum Boltzmann distribution. Performing a contour integral…

Chemical Physics · Physics 2016-02-03 Timothy J. H. Hele

Two-dimensional Raman and hybrid terahertz/Raman spectroscopic techniques provide invaluable insight into molecular structure and dynamics of condensed-phase systems. However, corroborating experimental results with theory is difficult due…

Chemical Physics · Physics 2022-04-13 Tomislav Begušić , Xuecheng Tao , Geoffrey A. Blake , Thomas F. Miller

A shadow molecular dynamics scheme for flexible charge models is presented, where the shadow Born-Oppenheimer potential is derived from a coarse-grained approximation of range-separated density functional theory. The interatomic potential,…

Chemical Physics · Physics 2023-07-27 James Goff , Yu Zhang , Christian F. A. Negre , Andrew Rohskopf , Anders M. N. Niklasson

With the continuous growth of processing power for scientific computing, first principles Born-Oppenheimer molecular dynamics (MD) simulations are becoming increasingly popular for the study of a wide range of problems in materials science,…

Materials Science · Physics 2015-06-04 Anders M. N. Niklasson , Marc J. Cawkwell

A thermodynamic system is driven into a nonequilibrium condition when a time-dependent force or a nonconservative force represented by a protocol $\lambda(t)$ is applied. Such a system is time irreversible in the sense that the motion under…

Statistical Mechanics · Physics 2014-06-03 Jae Dong Noh

A class of Brownian dynamics algorithms for stochastic reaction-diffusion models which include reversible bimolecular reactions is presented and analyzed. The method is a generalization of the $\lambda$--$\newrho$ model for irreversible…

Biological Physics · Physics 2010-05-12 J. Lipkova , K. C. Zygalakis , S. J. Chapman , R. Erban

A Lagrangian generalization of time-reversible Born-Oppenheimer molecular dynamics [Niklasson et al., Phys. Rev. Lett. vol. 97, 123001 (2006)] is proposed. The Lagrangian includes extended electronic degrees of freedom as auxiliary…

Materials Science · Physics 2008-03-08 Anders M. N. Niklasson

Ehrenfest, Born-Oppenheimer, Langevin and Smoluchowski dynamics are shown to be accurate approximations of time-independent Schr\"odinger observables for a molecular system avoiding caustics, in the limit of large ratio of nuclei and…

Mathematical Physics · Physics 2010-01-12 Anders Szepessy

A binary fluid mixture in contact with lateral particle reservoirs is considered. By imposing different particle concentrations in these reservoirs, the system can be maintained under controlled non-equilibrium conditions. Previous…

Statistical Mechanics · Physics 2026-04-01 O. Politano , Alejandro L. Garcia , F. Baras , M. Malek Mansour

Wavefunction extrapolation greatly reduces the number of self-consistent field (SCF) iterations and thus the overall computational cost of Born-Oppenheimer molecular dynamics (BOMD) that is based on the Kohn-Sham density functional theory.…

Computational Physics · Physics 2016-07-27 Jun Fang , Xingyu Gao , Haifeng Song , Han Wang

Time-reversal symmetry breaking (TRSB) has been central to detecting exotic phases of matter. Here, we leverage the circuit electrodynamics capabilities of superconducting devices to propose a novel scheme based on a multimode…

In this paper, we consider the time-dependent Born-Oppenheimer approximation (BOA) of a classical quantum molecule involving a possibly large number of nuclei and electrons, described by a Schr\"odinger equation. In the spirit of Born and…

Quantum Physics · Physics 2025-05-27 Sebastian Gherghe , Iván Moyano , Israel Michael Sigal
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