Chrome Extension
WeChat Mini Program
Use on ChatGLM

A Variational Approach to Assess Reaction Coordinates for Two-Step Crystallization.

Journal of chemical physics online/˜The œJournal of chemical physics/Journal of chemical physics(2023)

Cited 3|Views11
No score
Abstract
Molecule- and particle-based simulations provide the tools to test, in microscopic detail, the validity of classical nucleation theory. In this endeavor, determining nucleation mechanisms and rates for phase separation requires an appropriately defined reaction coordinate to describe the transformation of an out-of-equilibrium parent phase for which myriad options are available to the simulator. In this article, we describe the application of the variational approach to Markov processes to quantify the suitability of reaction coordinates to study crystallization from supersaturated colloid suspensions. Our analysis indicates that collective variables (CVs) that correlate with the number of particles in the condensed phase, the system potential energy, and approximate configurational entropy often feature as the most appropriate order parameters to quantitatively describe the crystallization process. We apply time-lagged independent component analysis to reduce high-dimensional reaction coordinates constructed from these CVs to build Markov State Models (MSMs), which indicate that two barriers separate a supersaturated fluid phase from crystals in the simulated environment. The MSMs provide consistent estimates for crystal nucleation rates, regardless of the dimensionality of the order parameter space adopted; however, the two-step mechanism is only consistently evident from spectral clustering of the MSMs in higher dimensions. As the method is general and easily transferable, the variational approach we adopt could provide a useful framework to study controls for crystal nucleation.
More
Translated text
Key words
Continuous Crystallization,Crystallization
AI Read Science
Must-Reading Tree
Example
Generate MRT to find the research sequence of this paper
Chat Paper
Summary is being generated by the instructions you defined