Research conducted in my group strives to elucidate the origins of molecular behavior by probing fundamental physical properties and chemical propensities. Ongoing experiments exploit diverse forms linear and nonlinear laser spectroscopy, many of which were pioneered in our laboratories (e.g., polarization-resolved resonant four-wave mixing and cavity ring-down polarimetry), to interrogate the ground-state and excited-state potential energy hypersurfaces of theoretically tractable species, thereby unraveling the intimate coupling among electronic, nuclear, isotopic, and environmental degrees of freedom that ultimately governs their structure and dynamics. When combined with synergistic computational analyses, such information affords a trenchant glimpse of phenomena that permeate the entire fabric of chemistry and impact upon frontier fields of molecular science, including the central concepts of chirality, proton transfer, non-covalent interactions, and solvation.