Artificial Photosynthetic Reaction Center Exhibiting Acid-Responsive Regulation of Photoinduced Charge Separation
- Arizona State Univ., Tempe, AZ (United States). School of Molecular Sciences
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and QB3 Inst.
Charge separation (CS) is the primary light-driven reaction in photosynthesis whereas onphotochemical quenching (NPQ) is a photoprotective regulatory mechanism employed by many photosynthetic organisms to dynamically modulate energy flow within the photosynthetic apparatus in response to fluctuating light conditions. Activated by decreases in lumen pH produced during periods of high photon flux, NPQ induces rapid thermal dissipation of excess excitation energy. As a result, the rate of CS decreases, thereby limiting the accumulation of potentially deleterious reactive intermediates and byproducts. In this article, a molecular triad that functionally mimics the effects of NPQ associated with an artificial photosynthetic reaction center is described. Steady-state absorption and emission, time-resolved fluorescence, and transient absorption spectroscopies have been used to demonstrate a 1 order of magnitude reduction in the CS quantum yield via reversible protonation of an excited-state-quenching molecular switch moiety. As in the natural system, the populations of unquenched and quenched states and therefore the overall yields of CS were found to be dependent on acid concentration.
- Research Organization:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC03-76F000098; AC02-05CH11231; FG02-03ER15393
- OSTI ID:
- 1378341
- Journal Information:
- Journal of Physical Chemistry. B, Vol. 120, Issue 40; ISSN 1520-6106
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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