Charge localization in multiply charged clusters and their electrical properties: Some insights into electrospray droplets

TL;DR

This study uses Monte Carlo simulations to explore how charge distribution and surface composition affect the electrical properties of charged Lennard-Jones clusters, revealing size-dependent behaviors akin to conductors or uniformly charged spheres.

Contribution

It provides new insights into the surface composition and electrical behavior of charged clusters across different sizes using advanced simulation techniques.

Findings

Charged particles preferentially occupy surface sites due to Coulomb repulsion.

Clusters behave as spherical conductors or uniformly charged spheres depending on size.

Full surface occupancy is rarely achieved below the stability limit.

Abstract

The surface composition of charged Lennard-Jones clusters A$_N^{n+}$, composed of N particles (55 \leq N \leq 1169) among which n are positively charged with charge q, thus having a net total charge Q = nq, is investigated by Monte Carlo with Parallel Tempering simulations. At finite temperature, the surface sites of these charged clusters are found to be preferentially occupied by charged particles carrying large charges, due to Coulombic repulsions, but the full occupancy of surface sites is rarely achieved for clusters below the stability limit defined in this work. Large clusters (N = 1169) follow the same trends, with a smaller propensity for positive particles to occupy the cluster surface at non-zero temperature. We show that these charged clusters rather behave as electrical spherical conductors for the smaller sizes (N \leq 147) but as spheres uniformly charged in their volume for the larger sizes (N = 1169).