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University of Pennsylvania

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J. Am. Chem. Soc., Publication Date (Web): August 22, 2018 | DOI: 10.1021/jacs.8b04593 Ultrafast Energy Transfer Involving the Red Chlorophylls of Cyanobacterial Photosystem I Probed through Two-Dimensional Electronic Spectroscopy

Yumin Lee^† , Michael Gorka^‡ , John H. Golbeck^‡§ , and Jessica M. Anna^*†^† Deparment of Chemistry, University of Pennsylvania, 231 South 34 Street, Philadelphia, Pennsylvania 19104, United States

^‡ Department of Biochemistry and Molecular Biology, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

^§Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

^*Corresponding Author

Abstract

Photosystem I (PSI) is a naturally occurring light-harvesting complex that drives oxygenic photosynthesis through a series of photoinitiated transmembrane electron transfer reactions that occur with a high quantum efficiency. Understanding the mechanism by which this process occurs is fundamental to understanding the near-unity quantum efficiency of PSI and in turn could lead to further insight into PSI-based technologies for solar energy conversion. In this article, we have applied two-dimensional electronic spectroscopy to PSI complexes isolated from two different cyanobacterial strains to gain further insight into the ultrafast energy transfer in PSI. The PSI complexes studied differ in the number and absorption of the red chlorophylls, chlorophylls that lie to lower energies than the reaction center. By applying a global analysis to the 2D electronic spectra of the PSI complexes we extract 2D decay associated spectra (2D-DAS). Through analysis of the 2D-DAS we observe a 50 fs relaxation among the bulk antenna chlorophylls in addition to two pathways of energy equilibration involving the red chlorophylls: a fast 200 fs equilibration followed by a 2-4 ps equilibration. As demonstrated with a model system, the λ₁, λ₃ coordinates of the cross-peaks in the 2D-DAS spectra indicate that the two equilibration pathways involve different chlorophyll molecules.

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형식Research article
게재일2018년 08월 (BRIC 등록일 2018-09-18)
연구진국외 연구진
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