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Extended Lagrangian Born–Oppenheimer molecular dynamics: from density functional theory to charge relaxation models

  • Topical Review - Computational Methods
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Abstract

We present a review of extended Lagrangian Born–Oppenheimer molecular dynamics and its most recent development. The molecular dynamics framework is first derived for general Hohenberg–Kohn density functional theory and it is then presented in explicit forms for thermal Hartree–Fock theory using a density matrix formalism, for self-consistent charge density functional tight-binding theory, and for general non-linear charge relaxation models that can be designed and optimized using modern machine learning methods. Our intention is to give a self-contained but brief and hopefully pedagogical presentation.

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Data Availability Statement

This manuscript has no associated data or the data will not be deposited. [Authors’ comment: Additional data or information can be made available by the author upon reasonable requests.]

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Acknowledgements

The author is indebted and grateful to a number of collaborators that have contributed to the development of XL-BOMD during the last decade of which most appear as co-authors of the XL-BOMD publications cited in this review. Some of those that do not appear as co-authors, but still have contributed through stimulating discussions and critical comments are Eric Chisolm, Jürg Hutter, Travis Peery, Kipton Barros, Linnea Andersson, Joshua Finkelstein, Vikram Gavini, Konstantin Leon, Mariana Rossi, Oscar Grånäs, Anders Bergman, and John Wills. This work is supported by the U.S. Department of Energy Office of Basic Energy Sciences (“Next generation quantum based molecular dynamics”, FWP LANLE8AN / KC0301061) and by the U.S. Department of Energy through the Los Alamos National Laboratory. Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy Contract No. 892333218NCA000001.

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    Anders M. N. Niklasson

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Niklasson, A.M.N. Extended Lagrangian Born–Oppenheimer molecular dynamics: from density functional theory to charge relaxation models. Eur. Phys. J. B 94, 164 (2021). https://doi.org/10.1140/epjb/s10051-021-00151-6

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