Room Temperature Dye Glasses: A Guideline Toward the Fabrication of Amorphous Dye Films with Monomeric Absorption and Emission

Abstract

The morphology of films containing photoactive materials is crucial for the performance of solid-state dye applications. Organic dyes tend to crystallize due to their usually planar molecular structure and the resulting intermolecular interactions. This leads to inhomogeneous films with crystalline, aggregated, and amorphous regions, decreasing device efficiency and complicating spectral analysis. Improving the glass-forming ability of organic dyes therefore presents a major challenge for solid-state dye applications. Here, we present a guideline to create organic dye glasses using BODIPY as a model dye. The method is based on the strategic design of BODIPY derivatives, equipped with short alkyl chains, in combination with blending of two or more derivatives. Mixing increases the entropy of the liquid state and lowers the thermodynamic driving force for crystallization as well as the kinetic fragility of the system. This enables the fabrication of homogeneous thin films without any additives. In these films, the dye molecules are trapped in a glassy state, featuring monomeric absorption and emission. This strategy leads to a BODIPY material with an amorphous character in thin films, dropcast films, and bulk. Further, the strategy is based on thermodynamics and is therefore expected to be general, enabling the transformation of any dye molecule into a glass former.