Functional Connectivity of Red Chlorophylls in Cyanobacterial Photosystem I Revealed by Fluence-Dependent Transient Absorption

Sohail, Sara H.; Sohoni, Siddhartha; Ting, Po-Chieh; Fantz, Lexi R.; Abdulhadi, Sami M.; MacGregor-Chatwin, Craig; Hitchcock, Andrew; Hunter, C. Neil; Engel, Gregory S.; Massey, Sara C.

doi:10.1021/acs.jpcb.5c00198

Title: Functional Connectivity of Red Chlorophylls in Cyanobacterial Photosystem I Revealed by Fluence-Dependent Transient Absorption

Journal Article · Tue Mar 18 00:00:00 UTC 2025 · Journal of Physical Chemistry. B

DOI: https://doi.org/10.1021/acs.jpcb.5c00198 · OSTI ID:2531272

^[1]; Sohoni, Siddhartha ^[2]; Ting, Po-Chieh ^[2];

^[3]; Abdulhadi, Sami M. ^[2]; MacGregor-Chatwin, Craig ^[4];

^[4];

^[2];

^[3]

University of Chicago, IL (United States); National Institutes of Health, Bethesda, MD (United States); Swarthmore College, PA (United States)
University of Chicago, IL (United States)
Southwestern University, Georgetown, TX (United States)
University of Sheffield (United Kingdom)

External stressors modulate the oligomerization state of photosystem I (PSI) in cyanobacteria. The number of red chlorophylls (Chls), pigments lower in energy than the P700 reaction center, depends on the oligomerization state of PSI. Here, we use ultrafast transient absorption spectroscopy to interrogate the effective connectivity of the red Chls in excitonic energy pathways in trimeric PSI in native thylakoid membranes of the model cyanobacterium Synechocystis sp. PCC 6803, including emergent dynamics, as red Chls increase in number and proximity. Fluence-dependent dynamics indicate singlet–singlet annihilation within energetically connected red Chl sites in the PSI antenna but not within bulk Chl sites on the picosecond time scale. These data support picosecond energy transfer between energetically connected red Chl sites as the physical basis of singlet–singlet annihilation. The time scale of this energy transfer is faster than predicted by Förster resonance energy transfer calculations, raising questions about the physical mechanism of the process. Our results indicate distinct strategies to steer excitations through the PSI antenna; the red Chls present a shallow reservoir that direct excitations away from P₇₀₀, extending the time to trapping by the reaction center.

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Research Organization:: Southwestern University, Georgetown, TX (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); Royal Society University Research Fellowship; USDOE Office of Science (SC), Basic Energy Sciences (BES); Vannevar Bush Faculty Fellowship program

Grant/Contract Number:: SC0001035; SC0020131

OSTI ID:: 2531272

Journal Information:: Journal of Physical Chemistry. B, Journal Name: Journal of Physical Chemistry. B Journal Issue: 12 Vol. 129; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Functional Connectivity of Red Chlorophylls in Cyanobacterial Photosystem I Revealed by Fluence-Dependent Transient Absorption

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