Thin Film Growth of Phase-Separating Phthalocyanine-Fullerene Blends: A Combined Experimental and Computational Study

TL;DR

This study investigates the growth mechanisms and morphologies of CuPc and C60 thin films, revealing temperature-dependent behaviors and providing insights into optimizing organic solar cell performance through combined experimental and computational approaches.

Contribution

It offers a detailed analysis of phase-separating blends' growth processes and morphologies, integrating real-time experiments with kinetic Monte-Carlo simulations for the first time.

Findings

Pure CuPc forms a smooth wetting layer before roughening.

C60 rapidly forms islands early in growth.

Higher temperature reduces island density and increases structural features.

Abstract

Blended organic thin films have been studied during the last decades due to their applicability in organic solar cells. Although their optical and electronic features have been examined intensively, there is still lack of detailed knowledge about their growth processes and resulting morphologies, which play a key role for the efficiency of optoelectronic devices such as organic solar cells. In this study, pure and blended thin films of copper phthalocyanine (CuPc) and the Buckminster fullerene (C60) were grown by vacuum deposition onto a native silicon oxide substrate at two different substrate temperatures, 310 K and 400 K. The evolution of roughness was followed by in-situ real-time X-ray reflectivity. Crystal orientation, island densities and morphology were examined after the growth by X-ray diffraction experiments and microscopy techniques. The formation of a smooth wetting layer followed by rapid roughening was found in pure CuPc thin films, whereas C60 shows a fast formation of distinct islands at a very early stage of growth. The growth of needle-like CuPc crystals loosing their alignment with the substrate was identified in co-deposited thin films. Furthermore, the data demonstrates that structural features become larger and more pronounced and that the island density decreases by a factor of four when going from 310 K to 400 K. Finally, the key parameters roughness and island density were well reproduced on a smaller scale by kinetic Monte-Carlo simulations of a generic, binary lattice model with simple nearest-neighbor interaction energies.