Multidimensional Electronic and Vibrational Spectroscopy: An Ultrafast Probe of Molecular Relaxation and Reaction Dynamics

Multidimensional optical spectroscopy in the visible and infra-red is a rapidly developing technique enabling direct observation of complex dynamics of molecules in complex environments such as liquids and proteins. Measuring the correlation between excited and detected frequencies with sub-picosecond resolution has enabled the resolution of long-standing problems such as energy transfer in photosynthesis and the life-sustaining structural rearrangements of liquid water. This chapter aims to provide a bridge between the concepts familiar in the AMO physics community and how those ideas and experimental methods are applied to condensed phase molecular spectroscopy, We outline the technical challenges of these powerful methods while considering a few examples of experiments that showcase the unique perspective offered by 2D electronic and vibrational spectroscopy.