Generalized extended Lagrangian Born-Oppenheimer molecular dynamics
Abstract
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 derived directly from the extended Lagrangian under the condition of an adiabatic separation between the nuclear and the electronic degrees of freedom. We show how this separation is automatically fulfilled and system independent. The generalized equations of motion require only one diagonalization per time step and are applicable to a broader range of materials with improved accuracy and stability compared to previous formulations.
- Authors:
-
- Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1184028
- Alternate Identifier(s):
- OSTI ID: 1212192; OSTI ID: 1416453
- Grant/Contract Number:
- AC52-06NA25396; FWP#LANL20101053
- Resource Type:
- Journal Article: Published Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Name: Journal of Chemical Physics Journal Volume: 141 Journal Issue: 16; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; molecular dynamics; Lagrangian mechanics; equations of motion; ground states; potential energy surfaces
Citation Formats
Niklasson, Anders M. N., and Cawkwell, Marc J. Generalized extended Lagrangian Born-Oppenheimer molecular dynamics. United States: N. p., 2014.
Web. doi:10.1063/1.4898803.
Niklasson, Anders M. N., & Cawkwell, Marc J. Generalized extended Lagrangian Born-Oppenheimer molecular dynamics. United States. https://doi.org/10.1063/1.4898803
Niklasson, Anders M. N., and Cawkwell, Marc J. 2014.
"Generalized extended Lagrangian Born-Oppenheimer molecular dynamics". United States. https://doi.org/10.1063/1.4898803.
@article{osti_1184028,
title = {Generalized extended Lagrangian Born-Oppenheimer molecular dynamics},
author = {Niklasson, Anders M. N. and Cawkwell, Marc J.},
abstractNote = {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 derived directly from the extended Lagrangian under the condition of an adiabatic separation between the nuclear and the electronic degrees of freedom. We show how this separation is automatically fulfilled and system independent. The generalized equations of motion require only one diagonalization per time step and are applicable to a broader range of materials with improved accuracy and stability compared to previous formulations.},
doi = {10.1063/1.4898803},
url = {https://www.osti.gov/biblio/1184028},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 16,
volume = 141,
place = {United States},
year = {Wed Oct 29 00:00:00 EDT 2014},
month = {Wed Oct 29 00:00:00 EDT 2014}
}
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1063/1.4898803
Other availability
Cited by: 42 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Energy conserving, linear scaling Born-Oppenheimer molecular dynamics
journal, October 2012
- Cawkwell, M. J.; Niklasson, Anders M. N.
- The Journal of Chemical Physics, Vol. 137, Issue 13
Molecular dynamics without effective potentials via the Car-Parrinello approach
journal, August 1990
- Remler, Dahlia K.; Madden, Paul A.
- Molecular Physics, Vol. 70, Issue 6
Extended Lagrangian Born–Oppenheimer molecular dynamics with dissipation
journal, June 2009
- Niklasson, Anders M. N.; Steneteg, Peter; Odell, Anders
- The Journal of Chemical Physics, Vol. 130, Issue 21
DFTB+, a Sparse Matrix-Based Implementation of the DFTB Method †
journal, July 2007
- Aradi, B.; Hourahine, B.; Frauenheim, Th.
- The Journal of Physical Chemistry A, Vol. 111, Issue 26
A class of methods for solving nonlinear simultaneous equations
journal, January 1965
- Broyden, C. G.
- Mathematics of Computation, Vol. 19, Issue 92
The accuracy of symplectic integrators
journal, March 1992
- McLachlan, R. I.; Atela, P.
- Nonlinearity, Vol. 5, Issue 2
Extended Born-Oppenheimer Molecular Dynamics
journal, March 2008
- Niklasson, Anders M. N.
- Physical Review Letters, Vol. 100, Issue 12
Fock matrix dynamics
journal, March 2004
- Pulay, Peter; Fogarasi, Géza
- Chemical Physics Letters, Vol. 386, Issue 4-6
Extended Lagrangian Born-Oppenheimer molecular dynamics in the limit of vanishing self-consistent field optimization
journal, December 2013
- Souvatzis, Petros; Niklasson, Anders M. N.
- The Journal of Chemical Physics, Vol. 139, Issue 21
Elliptic Preconditioner for Accelerating the Self-Consistent Field Iteration in Kohn--Sham Density Functional Theory
journal, January 2013
- Lin, Lin; Yang, Chao
- SIAM Journal on Scientific Computing, Vol. 35, Issue 5
Ab Initio Molecular Dynamics Simulations
journal, January 1996
- Tuckerman, Mark E.; Ungar, P. Jeffrey; von Rosenvinge, Tycho
- The Journal of Physical Chemistry, Vol. 100, Issue 31
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Time-Reversible Born-Oppenheimer Molecular Dynamics
journal, September 2006
- Niklasson, Anders M. N.; Tymczak, C. J.; Challacombe, Matt
- Physical Review Letters, Vol. 97, Issue 12
Self-consistent-charge density-functional tight-binding method for simulations of complex materials properties
journal, September 1998
- Elstner, M.; Porezag, D.; Jungnickel, G.
- Physical Review B, Vol. 58, Issue 11, p. 7260-7268
Simultaneous Relaxation of Nuclear Geometries and Electric Charge Densities in Electronic Structure Theories
journal, May 1983
- Bendt, Paul; Zunger, Alex
- Physical Review Letters, Vol. 50, Issue 21
Broyden's method for self-consistent field convergence acceleration
journal, April 1984
- Srivastava, G. P.
- Journal of Physics A: Mathematical and General, Vol. 17, Issue 6
Lagrangian formulation with dissipation of Born-Oppenheimer molecular dynamics using the density-functional tight-binding method
journal, July 2011
- Zheng, Guishan; Niklasson, Anders M. N.; Karplus, Martin
- The Journal of Chemical Physics, Vol. 135, Issue 4
\mathcal{O}(N) methods in electronic structure calculations
journal, February 2012
- Bowler, D. R.; Miyazaki, T.
- Reports on Progress in Physics, Vol. 75, Issue 3
Efficient and Accurate Car-Parrinello-like Approach to Born-Oppenheimer Molecular Dynamics
journal, February 2007
- Kühne, Thomas D.; Krack, Matthias; Mohamed, Fawzi R.
- Physical Review Letters, Vol. 98, Issue 6
Car-Parrinello molecular dynamics: Car-Parrinello molecular dynamics
journal, September 2011
- Hutter, Jürg
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 4
Crystal Structures of Zirconia from First Principles and Self-Consistent Tight Binding
journal, December 1998
- Finnis, M. W.; Paxton, A. T.; Methfessel, M.
- Physical Review Letters, Vol. 81, Issue 23
Symplectic integration of Hamiltonian systems
journal, May 1990
- Channell, P. J.; Scovel, C.
- Nonlinearity, Vol. 3, Issue 2
Simplified method for calculating the energy of weakly interacting fragments
journal, February 1985
- Harris, J.
- Physical Review B, Vol. 31, Issue 4
Higher-order symplectic integration in Born–Oppenheimer molecular dynamics
journal, December 2009
- Odell, Anders; Delin, Anna; Johansson, Börje
- The Journal of Chemical Physics, Vol. 131, Issue 24
A Self-Consistent Charge Density-Functional Based Tight-Binding Method for Predictive Materials Simulations in Physics, Chemistry and Biology
journal, January 2000
- Frauenheim, Th.; Seifert, G.; Elsterner, M.
- physica status solidi (b), Vol. 217, Issue 1
Analysis of Time Reversible Born-Oppenheimer Molecular Dynamics
journal, December 2013
- Lin, Lin; Lu, Jianfeng; Shao, Sihong
- Entropy, Vol. 16, Issue 1
Modified Broyden’s method for accelerating convergence in self-consistent calculations
journal, December 1988
- Johnson, D. D.
- Physical Review B, Vol. 38, Issue 18
Tight-binding models and density-functional theory
journal, June 1989
- Foulkes, W. Matthew C.; Haydock, Roger
- Physical Review B, Vol. 39, Issue 17
Computer Simulation of the Lattice Dynamics of Solids
journal, December 1969
- Dickey, J. M.; Paskin, Arthur
- Physical Review, Vol. 188, Issue 3
First principles molecular dynamics without self-consistent field optimization
journal, January 2014
- Souvatzis, Petros; Niklasson, Anders M. N.
- The Journal of Chemical Physics, Vol. 140, Issue 4
Accelerated, energy-conserving Born–Oppenheimer molecular dynamics via Fock matrix extrapolation
journal, January 2005
- Herbert, John M.; Head-Gordon, Martin
- Physical Chemistry Chemical Physics, Vol. 7, Issue 18
Monitoring energy drift with shadow Hamiltonians
journal, July 2005
- Engle, Robert D.; Skeel, Robert D.; Drees, Matthew
- Journal of Computational Physics, Vol. 206, Issue 2
Fast method for quantum mechanical molecular dynamics
journal, November 2012
- Niklasson, Anders M. N.; Cawkwell, Marc J.
- Physical Review B, Vol. 86, Issue 17
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138