We apply multiscale methods to describe the strained growth of multiple layers of C60 on a thin film of pentacene. We study this growth in the presence of a monolayer pentacene step to compare our simulations to recent experimental studies by Breuer and Witte of submonolayer growth in the presence of monolayer steps. The molecular-level details of this organic semiconductor interface have ramifications on the macroscale structural and electronic behavior of this system and allow us to describe several unexplained experimental observations for this system. The growth of a C60 thin film on a pentacene surface is complicated by the differing crystal habits of the two component species, leading to heteroepitactical growth. In order to probe this growth, we use three computational methods that offer different approaches to coarse-graining the system and differing degrees of computational efficiency. We present a new, efficient reaction-diffusion continuum model for 2D systems whose results compare well with mesoscale kinetic Monte Carlo (KMC) results for submonolayer growth. KMC extends our ability to simulate multiple layers but requires a library of predefined rates for event transitions. Coarse-grained molecular dynamics (CGMD) circumvents KMC's need for predefined lattices, allowing defects and grain boundaries to provide a more realistic thin film morphology. For multilayer growth, in this particularly suitable candidate for coarse-graining, CGMD is a preferable approach to KMC. Combining the results from these three methods, we show that the lattice strain induced by heteroepitactical growth promotes 3D growth and the creation of defects in the first monolayer. The CGMD results are consistent with experimental results on the same system by Conrad et al. and by Breuer and Witte in which C60 aggregates change from a 2D structure at low temperature to 3D clusters along the pentacene step edges at higher temperatures.

Two-dimensional covalent organic frameworks (COFs), with their predictable assembly into ordered porous crystalline materials, tunable composition, and high charge carrier mobility, offer the possibility of creating ordered bulk heterojunction solar cells given a suitable electron-transporting material to fill the pores. The photoconductive (hole-transporting) properties of many COFs have been reported, including the recent creation of a TT-COF/PCBM solar cell by Dogru et al. Although a prototype device has been fabricated, its poor solar efficiency suggests a potential issue with electron transport caused by the interior packing of the fullerenes. Such packing information is absent and cannot be obtained experimentally. In this paper, we use Kinetic Monte Carlo (KMC) simulations to understand the dominant pore-filling mechanisms and packing configurations of C60 molecules in a Pc-PBBA COF that are similar to the COF fabricated experimentally. The KMC simulations thus offer more realistic filling conditions than our previously used Monte Carlo (MC) techniques. We found persistently large separation distances between C60 molecules that are absent in the more tractable MC simulations and which are likely to hinder electron transport significantly. We attribute the looser fullerene packing to the existence of stable motifs with pairwise distances that are mismatched with the underlying adsorption lattice of the COF. We conclude that larger pore COFs may be necessary to optimize electron transport and hence produce higher efficiency devices.