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

Journal Article · · Journal of Chemical Theory and Computation
 [1]; ORCiD logo [1];  [2]
  1. Univ. of California, Berkeley, CA (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
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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.

Research Organization:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC52-06NA25396; AC02-05CH11231
OSTI ID:
1438113
Alternate ID(s):
OSTI ID: 1532299
Report Number(s):
LA-UR-17-29457
Journal Information:
Journal of Chemical Theory and Computation, Vol. 14, Issue 2; ISSN 1549-9618
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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Cited By (2)

Inertial extended-Lagrangian scheme for solving charge equilibration models journal January 2019
Inertial Extended-Lagrangian Scheme for Solving Charge Equilibration Models text January 2019

Figures / Tables (10)

Table 1(p. 4)table Table 1
Table 2(p. 5)table Table 2
Table 3(p. 6)table Table 3
Table 4(p. 7)table Table 4
Figure 1(p. 8)figure Figure 1
Figure 2(p. 9)figure Figure 2
Figure 3(p. 10)figure Figure 3
Figure 4(p. 11)figure Figure 4
Figure 5(p. 11)figure Figure 5
Figure B1(p. 13)figure Figure B1

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Mathematics
Molecular Dynamics
polarizable force fields