We present a free-energy driven kinetic Monte Carlo model to simulate homogeneous nucleation of metal nanoparticles (NPs) from vapor phase. The model accounts for monomer-cluster condensations, cluster–cluster collisions, and cluster evaporations simultaneously. Specifically, we investigate the homogeneous nucleation of Al NPs starting with different initial background temperatures. Our results indicate good agreement with earlier phenomenological studies using the Gibbs# free energy formulation from Classical Nucleation Theory (CNT). Furthermore, nucleation rates for various clusters are calculated through direct cluster observations. The steady-state nucleation rate estimated using two different approaches namely, the Yasuoka-Matsumoto (YM) and mean first passage time (MFPT) methods indicate excellent agreement with each other. Finally, our simulation results depict the expected increase in the entropy of mixing as clusters approach the nucleation barrier, followed by its subsequent drastic loss after the critical cluster formation resulting from first-order phase transitions. © 2017 American Institute of Chemical Engineers AIChE J, 2017

中文翻译：

---

气相合成过程中金属纳米粒子均匀成核的动力学蒙特卡洛模拟

我们提出了一种自由能驱动的动力学蒙特卡洛模型，以模拟气相中金属纳米颗粒（NPs）的均匀成核。该模型同时考虑了单体-团簇冷凝，团簇-团簇碰撞和团簇蒸发。具体来说，我们调查从不同的初始背景温度开始的Al NPs的均匀成核。我们的结果表明，与使用经典成核理论（CNT）的Gibbs＃自由能公式的早期现象学研究相吻合。此外，通过直接的星团观测可以计算出各种星团的成核率。使用Yasuoka-Matsumoto（YM）和平均首次通过时间（MFPT）方法这两种不同的方法估算的稳态成核率表明彼此之间的一致性很好。最后，我们的模拟结果表明，随着团簇接近成核壁垒，混合熵的预期增加，随后在由一阶相变导致的关键团簇形成之后，其随后的急剧损失。©2017美国化学工程师学会AIChE的Ĵ，2017年