Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Higher-Order Extended Lagrangian Born–Oppenheimer Molecular Dynamics for Classical Polarizable Models

Abstract

Generalized extended Lagrangian Born-Oppenheimer molecular dynamics (XLBOMD) methods provide a framework for fast iteration-free simulations of models that normally require expensive electronic ground state optimizations prior to the force evaluations at every time step. XLBOMD uses dynamically driven auxiliary degrees of freedom that fluctuate about a variationally optimized ground state of an approximate "shadow" potential which approximates the true reference potential. While the requirements for such shadow potentials are well understood, constructing such potentials in practice has previously been ad hoc, and in this work, we present a systematic development of XLBOMD shadow potentials that match the reference potential to any order. We also introduce a framework for combining friction-like dissipation for the auxiliary degrees of freedom with general-order integration, a combination that was not previously possible. These developments are demonstrated with a simple fluctuating charge model and point induced dipole polarization models.

Authors:
 [1]; ORCiD logo [1];  [2]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1438113
Alternate Identifier(s):
OSTI ID: 1532299
Report Number(s):
LA-UR-17-29457
Journal ID: ISSN 1549-9618
Grant/Contract Number:  
AC52-06NA25396; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Mathematics; Molecular Dynamics; polarizable force fields

Citation Formats

Albaugh, Alex, Head-Gordon, Teresa, and Niklasson, Anders M. N. Higher-Order Extended Lagrangian Born–Oppenheimer Molecular Dynamics for Classical Polarizable Models. United States: N. p., 2018. Web. doi:10.1021/acs.jctc.7b01041.
Copy to clipboard
Albaugh, Alex, Head-Gordon, Teresa, & Niklasson, Anders M. N. Higher-Order Extended Lagrangian Born–Oppenheimer Molecular Dynamics for Classical Polarizable Models. United States. https://doi.org/10.1021/acs.jctc.7b01041
Copy to clipboard
Albaugh, Alex, Head-Gordon, Teresa, and Niklasson, Anders M. N. Tue . "Higher-Order Extended Lagrangian Born–Oppenheimer Molecular Dynamics for Classical Polarizable Models". United States. https://doi.org/10.1021/acs.jctc.7b01041. https://www.osti.gov/servlets/purl/1438113.
Copy to clipboard
@article{osti_1438113,
title = {Higher-Order Extended Lagrangian Born–Oppenheimer Molecular Dynamics for Classical Polarizable Models},
author = {Albaugh, Alex and Head-Gordon, Teresa and Niklasson, Anders M. N.},
abstractNote = {Generalized extended Lagrangian Born-Oppenheimer molecular dynamics (XLBOMD) methods provide a framework for fast iteration-free simulations of models that normally require expensive electronic ground state optimizations prior to the force evaluations at every time step. XLBOMD uses dynamically driven auxiliary degrees of freedom that fluctuate about a variationally optimized ground state of an approximate "shadow" potential which approximates the true reference potential. While the requirements for such shadow potentials are well understood, constructing such potentials in practice has previously been ad hoc, and in this work, we present a systematic development of XLBOMD shadow potentials that match the reference potential to any order. We also introduce a framework for combining friction-like dissipation for the auxiliary degrees of freedom with general-order integration, a combination that was not previously possible. These developments are demonstrated with a simple fluctuating charge model and point induced dipole polarization models.},
doi = {10.1021/acs.jctc.7b01041},
journal = {Journal of Chemical Theory and Computation},
number = 2,
volume = 14,
place = {United States},
year = {Tue Jan 09 00:00:00 EST 2018},
month = {Tue Jan 09 00:00:00 EST 2018}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jctc.7b01041
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: Mth-order,more » $f(X)$, and Corresponding Variationally Minimized Set of Atomic Partial Charges, $q$, for That Order along with the Shadow Potential, U$d\atop{s}$$_{hadow}$, and Equations of Motion for Nuclear Degrees of Freedom and Auxiliary Matrix, mir̈i and mXẌ, Respectively« less
All figures and tables (10 total)
Save / Share:
Export Metadata
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:

Unified Approach for Molecular Dynamics and Density-Functional Theory
journal, November 1985

Molecular dynamics simulation of polarizable water by an extended Lagrangian method
journal, October 1992

Modeling induced polarization with classical Drude oscillators: Theory and molecular dynamics simulation algorithm
journal, August 2003

  • Lamoureux, Guillaume; Roux, Benoı̂t
  • The Journal of Chemical Physics, Vol. 119, Issue 6
  • DOI: 10.1063/1.1589749

Computer simulation of the dynamics of induced polarization fluctuations in water
journal, March 1991

Dynamical fluctuating charge force fields: Application to liquid water
journal, October 1994

  • Rick, Steven W.; Stuart, Steven J.; Berne, B. J.
  • The Journal of Chemical Physics, Vol. 101, Issue 7
  • DOI: 10.1063/1.468398

Development of an Accurate and Robust Polarizable Molecular Mechanics Force Field from ab Initio Quantum Chemistry
journal, January 2004

  • Kaminski, George A.; Stern, Harry A.; Berne, B. J.
  • The Journal of Physical Chemistry A, Vol. 108, Issue 4
  • DOI: 10.1021/jp0301103

Time-Reversible Born-Oppenheimer Molecular Dynamics
journal, September 2006

Time-reversible ab initio molecular dynamics
journal, April 2007

  • Niklasson, Anders M. N.; Tymczak, C. J.; Challacombe, Matt
  • The Journal of Chemical Physics, Vol. 126, Issue 14
  • DOI: 10.1063/1.2715556

Extended Born-Oppenheimer Molecular Dynamics
journal, March 2008

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
  • DOI: 10.1063/1.3148075

Geometric integration in Born-Oppenheimer molecular dynamics
journal, December 2011

  • Odell, Anders; Delin, Anna; Johansson, Börje
  • The Journal of Chemical Physics, Vol. 135, Issue 22
  • DOI: 10.1063/1.3660689

Fast method for quantum mechanical molecular dynamics
journal, November 2012

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
  • DOI: 10.1063/1.4834015

Generalized extended Lagrangian Born-Oppenheimer molecular dynamics
journal, October 2014

  • Niklasson, Anders M. N.; Cawkwell, Marc J.
  • The Journal of Chemical Physics, Vol. 141, Issue 16
  • DOI: 10.1063/1.4898803

Next generation extended Lagrangian first principles molecular dynamics
journal, August 2017

  • Niklasson, Anders M. N.
  • The Journal of Chemical Physics, Vol. 147, Issue 5
  • DOI: 10.1063/1.4985893

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
  • DOI: 10.1063/1.4862907

Geometric numerical integration illustrated by the Störmer–Verlet method
journal, May 2003

An efficient and stable hybrid extended Lagrangian/self-consistent field scheme for solving classical mutual induction
journal, November 2015

  • Albaugh, Alex; Demerdash, Omar; Head-Gordon, Teresa
  • The Journal of Chemical Physics, Vol. 143, Issue 17
  • DOI: 10.1063/1.4933375

Accurate Classical Polarization Solution with No Self-Consistent Field Iterations
journal, April 2017

  • Albaugh, Alex; Niklasson, Anders M. N.; Head-Gordon, Teresa
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 8
  • DOI: 10.1021/acs.jpclett.7b00450

Strong Analog Classical Simulation of Coherent Quantum Dynamics
journal, February 2017

Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory
journal, March 2017

  • Vitale, Valerio; Dziedzic, Jacek; Albaugh, Alex
  • The Journal of Chemical Physics, Vol. 146, Issue 12
  • DOI: 10.1063/1.4978684

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
  • DOI: 10.1063/1.3605303

Iterative Berechung der reziproken Matrix
journal, January 1933

  • Schulz, Günther
  • ZAMM - Zeitschrift für Angewandte Mathematik und Mechanik, Vol. 13, Issue 1
  • DOI: 10.1002/zamm.19330130111

Efficient treatment of induced dipoles
journal, August 2015

  • Simmonett, Andrew C.; Pickard, Frank C.; Shao, Yihan
  • The Journal of Chemical Physics, Vol. 143, Issue 7
  • DOI: 10.1063/1.4928530

An empirical extrapolation scheme for efficient treatment of induced dipoles
journal, October 2016

  • Simmonett, Andrew C.; Pickard, Frank C.; Ponder, Jay W.
  • The Journal of Chemical Physics, Vol. 145, Issue 16
  • DOI: 10.1063/1.4964866

A computer simulation method for the calculation of equilibrium constants for the formation of physical clusters of molecules: Application to small water clusters
journal, January 1982

  • Swope, William C.; Andersen, Hans C.; Berens, Peter H.
  • The Journal of Chemical Physics, Vol. 76, Issue 1
  • DOI: 10.1063/1.442716

The accuracy of symplectic integrators
journal, March 1992

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Inertial extended-Lagrangian scheme for solving charge equilibration models
    journal, January 2019

    • Leven, Itai; Head-Gordon, Teresa
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 34
    • DOI: 10.1039/c9cp02979f

    Inertial Extended-Lagrangian Scheme for Solving Charge Equilibration Models
    text, January 2019

      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Table 1 (p. 4)table
      Table 2 (p. 5)table
      Table 3 (p. 6)table
      Table 4 (p. 7)table
      Figure 1 (p. 8)figure
      Figure 2 (p. 9)figure
      Figure 3 (p. 10)figure
      Figure 4 (p. 11)figure
      Figure 5 (p. 11)figure
      Figure B1 (p. 13)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: