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Invited Lectures – 9 π 2011 Studies of Multichromophoric Systems by Two-dimensional Electronic Spectroscopy: Application to the Photosystem II Reaction Center Jennifer P. Ogilvie University of Michigan, Ann Arbor, USA �e photosystem II (PSII) reaction center is the heart of oxygenic photosynthesis, taking absorbed light from neighboring antenna complexes and creating a charge separation capable of spli�ing water. Despite the wealth of spectroscopic studies of the PSII reaction center, the basic energy transfer and charge separation dynamics remain poorly understood. With six chlorophyll a pigments and two pheophytins, the reaction center has a complex multichromophoric structure; similar pigment site energies and varying degrees of electronic coupling combine to create a broad linear absorption spectrum, making spectral assignments particularly difficult. In traditional nonlinear spectroscopy experiments, one must choose between temporal and spectral resolution, complicating the interpretation of these experiments. In addition, the degree of static disorder and electronic coupling in the system is difficult to discern. Two-dimensional electronic spectroscopy (2DES) overcomes many of these challenges, providing a more direct view of electronic coupling and femtosecond energy and charge dynamics. We present low-temperature 2DES data of the D1-D2-Cyt b559 reaction center complex from the femtosecond to the hundred picosecond timescale. We also present the decomposition of 2DES data into two-dimensional decay associated spectra (2D DAS), a method that characterizes the spectral signatures of energy and charge separation. Within this framework, we discuss the ultrafast energy and charge transfer dynamics of the PSII reaction center. A number of competing excitonic models for the PSII reaction center have been proposed in the literature. We present simulated 2D spectra based on these models for comparison with our 2DES data, and suggest possible refinements. Finally, we discuss future multidimensional spectroscopy experiments aimed at be�er separating signatures of energy and charge transfer. 38
π 2011 Invited Lectures – 9 Figure I9.1: 2DES spectra and simulations of the PSII RC at 77 K. Le�: at waiting time t2 = 28 fs, cross-peaks indicate excitonic coupling in the system. Middle: 2DES spectrum at waiting time t2 = 215 fs, showing growth of the cross-peak below the diagonal as energy is transferred to lower-lying electronic states. Right: simulated 2DES spectrum at waiting time t2 = 215 fs, based on a proposed exciton model for the PSII reaction center, using modified Redfield theory. N�� 39 Lectures
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