This document summarizes several scientific achievements: 1) Ultrafast hole transfer from a light absorber to a metal oxide nanoparticle catalyst for water oxidation was demonstrated for the first time across an ultrathin silica membrane, enabling efficient solar-powered water splitting. 2) A novel type of violaxanthin de-epoxidase enzyme was identified in green algae that is unrelated to the typical form found in plants but can still regulate photosynthesis. 3) Two-dimensional electronic-vibrational spectroscopy was used to directly track the flow of excitation energy through light harvesting complexes using local vibrations, without requiring a model.