Dissipative self-assembly of patchy particles under nonequilibrium drive: a computational study

TL;DR

This study uses computational simulations to demonstrate how nonequilibrium external forces can accelerate and stabilize the self-assembly of patchy particles, offering insights for designing advanced nanostructures.

Contribution

It introduces a computational framework analyzing the effects of external drives on dissipative self-assembly, revealing mechanisms to improve assembly speed and stability beyond equilibrium constraints.

Findings

External drives accelerate assembly kinetics.

External drives increase structural stability.

Validated results on larger systems of 100 particles.

Abstract

Inspired by biology and implemented using nanotechnology, the self-assembly of patchy particles has emerged as a pivotal mechanism for constructing complex structures that mimic natural systems with diverse functionalities. Here, we explore the dissipative self-assembly of patchy particles under nonequilibrium conditions, with the aim of overcoming the constraints imposed by equilibrium assembly. Utilizing extensive Monte Carlo (MC) and Molecular Dynamics (MD) simulations, we provide insight into the effects of external forces that mirror natural and chemical processes on the assembly rates and the stability of the resulting assemblies comprising $8$, $10$, and $13$ patchy particles. Implemented by a favorable bond-promoting drive in MC or a pulsed square wave potential in MD, our simulations reveal the role these external drives play in accelerating assembly kinetics and enhancing structural stability, evidenced by a decrease in the time to first assembly and an increase in the duration the system remains in an assembled state. Through the analysis of an order parameter, entropy production, bond dynamics, and interparticle forces, we unravel the underlying mechanisms driving these advancements. We also validated our key findings by simulating a larger system of $100$ patchy particles. Our comprehensive results not only shed light on the impact of external stimuli on self-assembly processes but also open a promising pathway for expanding the application by leveraging patchy particles for novel nanostructures.