TY - JOUR
T1 - Atomistic simulations of rare events using gentlest ascent dynamics
AU - Samanta, Amit
AU - Weinan, E.
N1 - Funding Information:
We acknowledge support by the Department of Energy under Grant No. de-sc0002623.
PY - 2012/3/28
Y1 - 2012/3/28
N2 - The dynamics of complex systems often involve thermally activated barrier crossing events that allow these systems to move from one basin of attraction on the high dimensional energy surface to another. Such events are ubiquitous, but challenging to simulate using conventional simulation tools, such as molecular dynamics. Recently, E and Zhou [Nonlinearity 24(6), 1831 (2011)]10.1088/0951- 7715/24/6/008 proposed a set of dynamic equations, the gentlest ascent dynamics (GAD), to describe the escape of a system from a basin of attraction and proved that solutions of GAD converge to index-1 saddle points of the underlying energy. In this paper, we extend GAD to enable finite temperature simulations in which the system hops between different saddle points on the energy surface. An effective strategy to use GAD to sample an ensemble of low barrier saddle points located in the vicinity of a locally stable configuration on the high dimensional energy surface is proposed. The utility of the method is demonstrated by studying the low barrier saddle points associated with point defect activity on a surface. This is done for two representative systems, namely, (a) a surface vacancy and ad-atom pair and (b) a heptamer island on the (111) surface of copper.
AB - The dynamics of complex systems often involve thermally activated barrier crossing events that allow these systems to move from one basin of attraction on the high dimensional energy surface to another. Such events are ubiquitous, but challenging to simulate using conventional simulation tools, such as molecular dynamics. Recently, E and Zhou [Nonlinearity 24(6), 1831 (2011)]10.1088/0951- 7715/24/6/008 proposed a set of dynamic equations, the gentlest ascent dynamics (GAD), to describe the escape of a system from a basin of attraction and proved that solutions of GAD converge to index-1 saddle points of the underlying energy. In this paper, we extend GAD to enable finite temperature simulations in which the system hops between different saddle points on the energy surface. An effective strategy to use GAD to sample an ensemble of low barrier saddle points located in the vicinity of a locally stable configuration on the high dimensional energy surface is proposed. The utility of the method is demonstrated by studying the low barrier saddle points associated with point defect activity on a surface. This is done for two representative systems, namely, (a) a surface vacancy and ad-atom pair and (b) a heptamer island on the (111) surface of copper.
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U2 - 10.1063/1.3692803
DO - 10.1063/1.3692803
M3 - Article
C2 - 22462832
AN - SCOPUS:84859524657
SN - 0021-9606
VL - 136
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 12
M1 - 124104
ER -