Comparative study on methodology in molecular dynamics simulation of nucleation

Abstract

Gas-liquid nucleation of 1000 Lennard-Jones atoms is simulated to evaluate temperature regulation methods and methods to obtain nucleation rate. The Berendsen and the Andersen thermostats are compared. The Berendsen thermostat is unable to control the temperature of clusters larger than the critical size. Independent of the thermostating method the velocities of individual atoms and the translational velocities of clusters up to at least six atoms are accurately described by the Maxwell velocity distribution. Simulations with the Andersen thermostat yield about two times higher nucleation rates than those with the Berendsen thermostat. Nucleation rate is extracted from the simulations by direct observation of times of nucleation onset and by the method of Yasuoka and Matsumoto [J. Chem. Phys. 109, 8451 (1998)]. Compared to the direct observation, the nucleation rates obtained from the method of Yasuoka and Matsumoto are higher by a factor of 3.