TY - JOUR
T1 - Constant pressure ab initio molecular dynamics with discrete variable representation basis sets
AU - Ma, Zhonghua
AU - Tuckerman, Mark
N1 - Funding Information:
The authors thank Hee-Seung Lee for many useful discussions. This work was supported by NSF CHE-0704036 and DOE FG05-08OR23334.
PY - 2010/11/14
Y1 - 2010/11/14
N2 - The use of discrete variable representation (DVR) basis sets within ab initio molecular dynamics calculations allows the latter to be performed with converged energies and, more importantly, converged forces. In this paper, we show how to carry out ab initio molecular dynamics calculations in the isothermal-isobaric ensemble with fully flexible simulation boxes within the DVR basis set framework. In particular, we derive the appropriate DVR based expression for the pressure tensor when the electronic structure is represented using Kohn-Sham density functional theory, and we examine the convergence of this expression as a function of the basis set size. An illustrative example using 64 silicon atoms in a fully flexible box using a combination of the Martyna-Tobias-Klein [Martyna, J. Chem. Phys. 101, 4177 (1994)] and Car-Parrinello [Car and Parinello, Phys. Rev. Lett. 55, 2471 (1985)] algorithms is presented to demonstrate the efficacy of the approach.
AB - The use of discrete variable representation (DVR) basis sets within ab initio molecular dynamics calculations allows the latter to be performed with converged energies and, more importantly, converged forces. In this paper, we show how to carry out ab initio molecular dynamics calculations in the isothermal-isobaric ensemble with fully flexible simulation boxes within the DVR basis set framework. In particular, we derive the appropriate DVR based expression for the pressure tensor when the electronic structure is represented using Kohn-Sham density functional theory, and we examine the convergence of this expression as a function of the basis set size. An illustrative example using 64 silicon atoms in a fully flexible box using a combination of the Martyna-Tobias-Klein [Martyna, J. Chem. Phys. 101, 4177 (1994)] and Car-Parrinello [Car and Parinello, Phys. Rev. Lett. 55, 2471 (1985)] algorithms is presented to demonstrate the efficacy of the approach.
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U2 - 10.1063/1.3499812
DO - 10.1063/1.3499812
M3 - Article
C2 - 21073216
AN - SCOPUS:78449296306
SN - 0021-9606
VL - 133
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 18
M1 - 184110
ER -