Probing Photosynthetic Energy and Charge Transfer with Two-Dimensional Electronic Spectroscopy.
Two-dimensional electronic spectroscopy (2DES) has emerged as a powerful method for elucidating the structure-function relationship in photosynthetic systems. In this Perspective, we discuss features of two-dimensional spectroscopy that make it highly suited to address questions about the underlying electronic structure that guides energy- and charge-transfer processes in light-harvesting materials. We briefly describe a pulse-shaping-based implementation of two-dimensional spectroscopy that is making the method widely accessible to problems spanning frequency regimes from the ultraviolet to the mid-infrared. We illustrate the utility of 2DES in the context of our recent studies of the primary energy-transfer and charge separation events in the photosystem II reaction center, discussing remaining challenges and speculating about exciting future directions for the field of multidimensional spectroscopy.
Department of Physics and Biophysics, University of Michigan, Ann Arbor, Michigan 48109-1040, United States.
Kristin L M
KL
Lewis
Department of Physics and Biophysics, University of Michigan, Ann Arbor, Michigan 48109-1040, United States.
Jennifer P
JP
Ogilvie