Bratschi Christoph, Huber Hanspeter
Departement Chemie, Universität Basel, Klingelbergstrasse 80, CH-4056 Basel, Switzerland.
J Chem Phys. 2007 Apr 28;126(16):164104. doi: 10.1063/1.2720832.
In this paper (paper I) and the following paper (paper II) [C. Bratschi, H. Huber, and D. J. Searles, J. Chem. Phys. 126, 164105 (2007)], a new molecular dynamics algorithm implementing the Gibbs ensemble will be presented and then on applied to the liquid-vapor coexistence curve for two ab initio CO2 potentials. In paper I, the Gibbs ensemble molecular dynamics algorithm using non-Hamiltonian molecular dynamics techniques is introduced. It is shown that states of the correct probability density function are sampled and the correct exchange probability is generated. The extended system Nose-Hoover formalism is used to generate a constant temperature ensemble with equal pressures in the subsystems, combined with single particle transfers between the subsystems, over several time steps, to get equal chemical potentials.
在本文（论文I）以及后续论文（论文II）[C. 布拉奇、H. 胡贝尔和D. J. 西尔斯，《化学物理杂志》126, 164105 (2007)]中，将提出一种实现吉布斯系综的新分子动力学算法，然后将其应用于两种从头算二氧化碳势的液 - 气共存曲线。在论文I中，引入了使用非哈密顿分子动力学技术的吉布斯系综分子动力学算法。结果表明，正确概率密度函数的状态被采样，并且产生了正确的交换概率。扩展系统的诺思 - 胡佛形式主义用于在子系统中生成具有相等压力的恒温系综，并结合子系统之间的单粒子转移，经过几个时间步长，以获得相等的化学势。
