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We present an efficient general approach to first principles molecular dynamics simulations based on extended Lagrangian Born-Oppenheimer molecular dynamics in the limit of vanishing self-consistent field optimization. The reduction of the…

Chemical Physics · Physics 2013-12-09 Petros Souvatzis , Anders M. N. Niklasson

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

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 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

Extended Lagrangian Born-Oppenheimer molecular dynamics based on Kohn-Sham density functional theory is generalized in the limit of vanishing self-consistent field optimization prior to the force evaluations. The equations of motion are…

Chemical Physics · Physics 2015-06-23 Anders M. N. Niklasson , Marc J. Cawkwell

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

Extended Lagrangian Born-Oppenheimer molecular dynamics [{\em Phys.\ Rev.\ Lett.\ } {\bf 2008}, {\em 100}, 123004] is presented for Hartree-Fock theory, where the extended electronic degrees of freedom are represented by a density matrix,…

Computational Physics · Physics 2020-05-29 Anders M. N. Niklasson

Extended Lagrangian Born-Oppenheimer molecular dynamics [Niklasson, Phys. Rev. Lett. 100 123004 (2008)] has been generalized to the propagation of the electronic wavefunctions. The technique allows highly efficient first principles…

Materials Science · Physics 2011-10-07 Peter Steneteg , Igor A. Abrikosov , Valery Weber , Anders M. N. Niklasson

We present an improved field-theoretic approach to the grand-canonical potential suitable for linear scaling molecular dynamics simulations using forces from self-consistent electronic structure calculations. It is based on an exact…

Computational Physics · Physics 2014-06-23 Dorothee Richters , Thomas D. Kühne

A method for carrying out semiclassical initial value representation calculations using first-principles molecular dynamics (FP-SC-IVR) is presented. This method can extract the full vibrational power spectrum of carbon dioxide from a…

Materials Science · Physics 2009-06-14 Michele Ceotto , Sule Atahan , Sangwoo Shim , Gianfranco Tantardini , Alán Aspuru-Guzik

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

Extended free energy Lagrangians are proposed for first principles molecular dynamics simulations at finite electronic temperatures for plane-wave pseudopotential and local orbital density matrix based calculations. Thanks to the extended…

Chemical Physics · Physics 2011-11-02 Anders M. N. Niklasson , Peter Steneteg , Nicolas Bock

We present a generalization of Extended Lagrangian Born-Oppenheimer molecular dynamics [Phys. Rev. Lett. vol. 100, 123004 (2008); Eur. Phys. J. B vol. 94, 164 (2021)] that also includes the electronic spin-degrees of freedom as extended…

Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) [Phys. Rev. Lett. vol. 100, 123004 (2008)] is combined with Kohn-Sham density functional theory (DFT) using a DFT+U correction based on the Hubbard model. This combined…

An accurate and easily extendable method to deal with lattice dynamics of solids is offered. It is based on first-principles molecular dynamics simulations and provides a consistent way to extract the best possible harmonic - or higher…

Materials Science · Physics 2013-10-14 Olle Hellman , I. A. Abrikosov , S. I. Simak

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

Classical molecular dynamics simulations have recently become a standard tool for the study of electrochemical systems. State-of-the-art approaches represent the electrodes as perfect conductors, modelling their responses to the charge…

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

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

The recent progress of linear-scaling or O(N) methods in the density functional theory (DFT) is remarkable. We expect that first-principles molecular dynamics (FPMD) simulations based on DFT can now treat more realistic and complex systems…

Materials Science · Physics 2014-11-11 Michiaki Arita , David R. Bowler , Tsuyoshi Miyazaki
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