Kraska T
Physical Chemistry, University of Cologne, Luxemburger Strasse 116, D-50939 Köln, Germany.
J Chem Phys. 2006 Feb 7;124(5):054507. doi: 10.1063/1.2162882.
The possibility to conduct simulations of homogeneous nucleation of argon from a supersaturated vapor phase using a microcanonical or NVE ensemble is evaluated (NVE: number of particles N, volume V, and energy E are constant). In order to initiate a phase separation kinetic energy is removed from the system in one step which transfers the system into a supersaturated state. After this temperature jump the simulation is continued in a NVE ensemble. The simulations are performed for different initial-state points and different temperature jumps. The cluster formation and growth over the course of the adiabatic simulations are analyzed. The progression of the temperature being related to the cluster size in NVE systems is traced. Also the influence of the size of the simulation system is investigated. For a certain range of low supersaturation a dynamic coexistence between two states has been found. Furthermore, the obtained nucleation rates are correlated with two simple functions. By applying the nucleation theorems to these functions the size and excess energy of the critical cluster are estimated. The results are consistent with other theoretical data and experimental data available in the literature.
评估了使用微正则系综或NVE系综（NVE：粒子数N、体积V和能量E恒定）对氩从过饱和气相进行均匀成核模拟的可能性。为了引发相分离，在一步中将动能从系统中移除，这会使系统转变为过饱和状态。在这个温度跳跃之后，模拟在NVE系综中继续进行。针对不同的初始状态点和不同的温度跳跃进行模拟。分析了绝热模拟过程中的团簇形成和生长。追踪了NVE系统中与团簇大小相关的温度变化过程。还研究了模拟系统大小的影响。对于一定范围的低过饱和度，发现了两种状态之间的动态共存。此外，将获得的成核速率与两个简单函数相关联。通过将成核定理应用于这些函数，估计了临界团簇的大小和过剩能量。结果与文献中其他理论数据和实验数据一致。
