A variational approach to nucleation simulation

被引：13

作者：

Piaggi, Pablo M. ^{[1
,3
]}

Valsson, Omar ^{[2
,3
]}

Parrinello, Michele ^{[2
,3
]}

机构：

[1] Ecole Polytech Fed Lausanne, Theory & Simulat Mat THEOS, USI Campus,Via Giuseppe Buffi 13, CH-6900 Lugano, Switzerland

[2] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, USI Campus,Via Giuseppe Buffi 13, CH-6900 Lugano, Switzerland

[3] USI, Natl Ctr Computat Design & Discovery Novel Mat MA, Fac Informat, Inst Sci Computaz, Via Giuseppe Buffi 13, CH-6900 Lugano, Switzerland

来源：

FARADAY DISCUSSIONS | 2016年 / 195卷

关键词：

MONTE-CARLO SIMULATIONS; MOLECULAR-DYNAMICS; LIQUID NUCLEATION; TRANSITIONS;

D O I：

10.1039/c6fd00127k

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We study by computer simulation the nucleation of a supersaturated Lennard-Jones vapor into the liquid phase. The large free energy barriers to transition make the time scale of this process impossible to study by ordinary molecular dynamics simulations. Therefore we use a recently developed enhanced sampling method [Valsson and Parrinello, Phys. Rev. Lett. 113, 090601 (2014)] based on the variational determination of a bias potential. We differ from previous applications of this method in that the bias is constructed on the basis of the physical model provided by the classical theory of nucleation. We examine the technical problems associated with this approach. Our results are very satisfactory and will pave the way for calculating the nucleation rates in many systems.

引用

页码：557 / 568

页数：12

共 30 条

[1]

[Anonymous], 2013, ADV NEURAL INFORM PR

[2]

[Anonymous], 2001, UNDERSTANDING MOL SI

[3] Transition path sampling: Throwing ropes over rough mountain passes, in the dark [J].