The Role of Solvent Fluctuations in Hydrophobic Assembly

TL;DR

This paper investigates how solvent fluctuations influence hydrophobic assembly, revealing that vapor tunnel formation accelerates particle assembly and demonstrating a broadly applicable methodology using transition path sampling.

Contribution

It introduces a methodology combining coarse-grained solvent modeling and transition path sampling to elucidate solvent roles in hydrophobic assembly.

Findings

Solvent fluctuations significantly impact assembly dynamics.

Vapor tunnel formation accelerates hydrophobic particle assembly.

The methodology is broadly applicable to similar systems.

Abstract

We use a coarse grained solvent model to study the self assembly of two nano-scale hydrophobic particles in water. We show how solvent degrees of freedom are involved in the process. By using tools of transition path sampling, we elucidate the reaction coordinates describing the assembly. In accord with earlier expectations, we find that fluctuations of the liquid-vapor-like interface surrounding the solutes are significant, in this case leading to the formation of a vapor tunnel between the two solute particles. This tunnel accelerates assembly. While considering this specific model system, the approach we use illustrates a methodology that is broadly applicable.