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Title: Temperature dependence of antenna excitation transport in native photosystem I particles. [Electronic energy transport (EET)]

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100163a047· OSTI ID:6125383

The temperature dependence of polarized photobleaching dynamics was investigated through 680-nm pump-probe experiments in the Chl a antenna of native photosystem 1 particles (Chl/P700 {approximately} 200) from spinach. The anisotropic decay time is lengthened by an order of magnitude (from {approximately}7 to {approximately}62 ps) when the temperature is reduced from 290 to 38 K; most of this increase occurs between 65 and 38 K. The occurrence of this transition temperature in the tens of kelvin reflects the participation of protein phonons in antenna EET. The isotopic decay kinetics are considerably less temperature sensitive, indicating that the anisotropic and isotropic decays stem from different energy-transfer processes with contrasting temperature dependence. The 38 K photobleaching spectrum at 5 ps exhibits considerably more weighting in the lower energy Chl a spectral forms than the room-temperature spectrum, suggesting that rapid spectral equilibration occurs in the photosystem 1 antenna. In light of the phonon frequency and electron-phonon coupling parameters determined in independent PSI-200 spectral hole-burning experiments, the quantitative temperature dependence int he anisotropic decay times is consistent with a theory for phonon-assisted EET in which the pertinent phonons are independent modes localized about the donor and acceptor chromophores.

DOE Contract Number:
W-7405-ENG-82
OSTI ID:
6125383
Journal Information:
Journal of Physical Chemistry; (United States), Vol. 95:10; ISSN 0022-3654
Country of Publication:
United States
Language:
English