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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 [{\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 [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 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 (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…

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 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

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 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…

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 introduce a new approach to density functional theory based on kinetic theory, showing that the Kohn-Sham equations can be derived as a macroscopic limit of a suitable Boltzmann kinetic equation in the limit of small mean free path…

Chemical Physics · Physics 2015-06-15 M. Mendoza , S. Succi , H. J. Herrmann

Newtonian physics is describes macro-objects sufficiently well, however it does not describe microobjects. A model of Extended Mechanics for Quantum Theory is based on an axiomatic generalization of Newtonian classical laws to arbitrary…

Classical Physics · Physics 2013-07-11 Timur F. Kamalov

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

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

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

The so-called Born-Huang ansatz is a fundamental tool in the context of ab-initio molecular dynamics, viz., it allows to effectively separate fast and slow degrees of freedom and thus treating electrons and nuclei at different mathematical…

Mesoscale and Nanoscale Physics · Physics 2023-01-24 Devashish Pandey , Xavier Oriols , Guillermo Albareda

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

Non-adiabatic molecular phenomena, arising from the breakdown of the Born-Oppenheimer approximation, govern the fate of virtually all photo-physical and photochemical processes and limit the quantum efficiency of molecules and other…

Quantum Physics · Physics 2024-05-15 N. S. Bassler , M. Reitz , R. Holzinger , A. Vibók , G. J. Halász , B. Gurlek , C. Genes

A simple formal procedure makes the main properties of the lagrangian binomial extendable to functions depending to any kind of order of the time--derivatives of the lagrangian coordinates. Such a broadly formulated binomial can provide the…

Classical Physics · Physics 2018-02-15 Federico Talamucci

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
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