Scaling in reversible submonolayer deposition

TL;DR

This paper investigates the scaling behavior of island and monomer densities, capture zone distributions, and island size distributions in reversible submonolayer growth using the Clarke-Vvedensky model, revealing multiple regimes and crossover phenomena.

Contribution

It extends rate-equation approaches for irreversible aggregation to predict scaling regimes in reversible growth, incorporating lattice effects and recurrence properties of random walks.

Findings

Identification of multiple scaling regimes with crossovers at different temperatures

Observation of Gaussian and bimodal distributions in capture zones and island sizes

Validation of the Pimpinelli-Einstein approach for reversible growth models

Abstract

The scaling of island and monomer density, capture zone distributions (CZDs), and island size distributions (ISDs) in reversible submonolayer growth was studied using the Clarke-Vvedensky model. An approach based on rate-equation results for irreversible aggregation (IA) models is extended to predict several scaling regimes in square and triangular lattices, in agreement with simulation results. Consistently with previous works, a regime I with fractal islands is observed at low temperatures, corresponding to IA with critical island size i=1, and a crossover to a second regime appears as the temperature is increased to \epsilon R^{2/3} ~ 1, where \epsilon is the single bond detachment probability and R is the diffusion-to-deposition ratio. In the square (triangular) lattice, a regime with scaling similar to IA with i=3 (i=2) is observed after that crossover. In the triangular lattice, a subsequent crossover to an IA regime with i=3 is observed, which is explained by the recurrence properties of random walks in two dimensional lattices, which is beyond the mean-field approaches. At high temperatures, a crossover to a fully reversible regime is observed, characterized by a large density of small islands, a small density of very large islands, and total island and monomer densities increasing with temperature, in contrast to IA models. CZDs and ISDs with Gaussian right tails appear in all regimes for R ~ 10^7 or larger, including the fully reversible regime, where the CZDs are bimodal. This shows that the Pimpinelli-Einstein (PE) approach for IA explains the main mechanisms for the large islands to compete for free adatom aggregation in the reversible model, and may be the reason for its successful application to a variety of materials and growth conditions.