Organic electronic materials are certain to be used in future low-cost lighting and energy harvesting devices. Inter-molecular interactions drive organic thin-film materials to form highly ordered morphologies when processed from solution or physical vapor. As a result, intra- and inter-molecular optical excitations (excitons) are aligned along different directions, leading to strong optical anisotropies. We are interested in investigating the inherent relationship between morphology and optical properties of organic materials and devices. For instance, we recently demonstrated a novel spectroscopic method that allows for independent determination of the dipole strengths, spectra, and dynamics of intra- and inter-molecular luminescent and absorbing excitons. Studies like these will inform a fundamental understanding of organic optoelectronic materials, suggest device architectures that exploit optical anisotropies for enhanced performance, and enable new methods to characterize structure via optical measurements. Ultimately, we aim to develop the methods, models, and materials necessary for understanding and quantifying the relationship between organic thin-film morphology and optical properties with ultrahigh spatial (10s of nm) and temporal (10s of fs) resolution.