8 research outputs found

    Observations of Coherence in Oxygenic Photosynthesis.

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    The field of two dimensional electronic spectroscopy (2DES) is rapidly advancing, both in theory and implementation to tackle increasingly complex and delicate problems. In the past seven years, observations of coherent or wave-like dynamics in 2D spectra of photosynthetic antenna has captured the imagination of many practitioners in the field, from theorists to experimentalists. Two questions are being raised: what is the origin of coherent dynamics in photosynthesis and, more importantly, do they matter for the function of biological systems? For certain photosynthetic antenna systems there is now considerable evidence and theoretical backing to suggest that coherent dynamics have a positive functional impact on energy transfer. Less explored is how such dynamics may influence charge separation, the primary purpose of photosynthetic reaction centers. Coherent signals are typically weak and difficult to resolve from population dynamics. To address this issue, we developed a method to collect 2DES which has dramatically improved the signal to noise over previous implementations. The new method has been applied to the photosystem II reaction center (PSII RC). The PSII RC is the photosynthetic enzyme uniquely capable of using solar energy to split water. As such it is an important system both for basic plant science and renewable energy generation. With this technique, we find eight coherent modes in PSII RC in the first such report of coherent dynamics on this system. Most of the wave-like motions are assigned to be of vibrational character while four are assigned to a mixture of vibrational and electronic character. Based on supporting simulations it is shown that charge separation is enhanced by the inclusion of such mixed character modes.PhDBiophysicsUniversity of Michigan, Horace H. Rackham School of Graduate Studieshttp://deepblue.lib.umich.edu/bitstream/2027.42/109003/1/fullerf_1.pd
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