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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

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

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 [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

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

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

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…

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…

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

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

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

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 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 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

We demonstrate the applicability of extended Lagrangian Born-Oppenheimer quantum-based molecular dynamics (XL-BOMD) to model electron transfer reactions occurring on solid-liquid interfaces. Specifically, we consider the reduction of O$_2$…

Within the nuclear-electronic orbital (NEO) framework, the real-time NEO time-dependent density functional theory (RT-NEO-TDDFT) approach enables the simulation of coupled electronic-nuclear dynamics. In this approach, the electrons and…

Chemical Physics · Physics 2023-03-22 Tao E. Li , Sharon Hammes-Schiffer

Graph-based linear scaling electronic structure theory for quantum-mechanical molecular dynamics simulations is adapted to the most recent shadow potential formulations of extended Lagrangian Born-Oppenheimer molecular dynamics, including…

Chemical Physics · Physics 2023-03-08 Christian F. A. Negre , Michael E. Wall , Anders M. N. Niklasson

We analyze the time reversible Born-Oppenheimer molecular dynamics (TRBOMD) scheme, which preserves the time reversibility of the Born-Oppenheimer molecular dynamics even with non-convergent self-consistent field iteration. In the linear…

Numerical Analysis · Mathematics 2015-06-16 Lin Lin , Jianfeng Lu , Sihong Shao

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 description is presented which can be used in conjunction with particle interpretations of quantum mechanics. A special example of such an interpretation is the well-known Bohm model. The Lagrangian density introduced here also…

Quantum Physics · Physics 2019-11-26 Roderick Sutherland
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