Quantifying reversibility in a phase-separating lattice gas: an analogy with self-assembly

Abstract

We present dynamic measurements of a lattice gas during phase separation, which we use as an analogy for self-assembly of equilibrium ordered structures. We use two approaches to quantify the degree of reversibility of this process: First, we count events in which bonds are made and broken; second, we use correlation-response measurements and fluctuation-dissipation ratios to probe reversibility during different time intervals. We show how correlation and response functions can be related directly to microscopic (ir)reversibility and we discuss the time dependence and observable dependence of these measurements, including the role of fast and slow degrees of freedom during assembly.