Evolution of pore structure in nanoparticle deposits from unimodal to bimodal pore size distributions: Focus on structural features of dendritic structures

Abstract

Nanoparticle deposits can exhibit various structures, including compact and dendritic structures, depending on the deposition conditions. While previous studies have characterized deposit structures using factors such as porosity and spatial autocorrelation index, the pore size distribution (PSD), which is an essential structural property, has only been explored in compact structures. In this study, we investigate the PSDs of the entire nanoparticle deposits, ranging from compact to dendritic structures. Deposits are formed using an off-lattice Monte Carlo simulation, and deposition conditions are represented by two dimensionless numbers (KnD, χF). The diffusive Knudsen number (KnD) ranges from 10−1.5 to 101.5, while the dimensionless translational energy of a particle (χF) ranges from 10−3 to 101.5. We use the Delaunay triangulation algorithm for fast PSD calculation, and validate the calculation method using theoretical values of ideal structures and experimental literature data. Our results show that bimodal PSDs appear under thermally-dominated conditions with high values of KnD, while unimodal PSDs with a constant mode radius (∼2.5 rp) are observed under highly advective conditions with high values of χF. We present the geometric mean radii and mode radii of pores as color-filled contours to show their variation trends with KnD and χF. Additionally, we propose a simple model that predicts dendrite width by combining the overall porosity and mode radii of pores. Our model's predictions reasonably match the dendrite width data obtained using a density-based clustering algorithm.