Molecular evolution enables proteins to acquire new functions beyond their original roles. We focus on a group of proteins that originally catalyzed DNA repair but have since evolved to perform functions such as circadian rhythm regulation and geomagnetic sensing. Using advanced spectroscopic techniques, including time-resolved vibrational spectroscopy, we study the molecular mechanisms behind this functional diversification and how amino acid substitutions affect protein functionality. Insights from this work may contribute to protein design with tailored functions.