Excitation transport and trapping on spectrally disordered lattices.

Abstract:

:It is widely assumed that the decay of fluorescence in photosynthetic systems can be described as a sum of exponential components and that the amplitude of each component is directly related to the absorption cross-section of the antenna pigments coupled to the fluorescing species. We present exact calculations of excited state decay in two-dimensional regular lattices of different geometries containing multiple spectral forms of antenna pigments. We illustrate by these calculations that there is no simple relation between the decay amplitudes (and resulting time-resolved excitation spectra) and the steady-state absorption spectra. Only in the limit that the electronic excitations reach a rapid equilibrium among all antenna spectral forms does the excitation spectrum depend uniquely on the spectral features of the array. Using the simulations in conjunction with our recent fluorescence studies, we examine excitation transport and trapping dynamics in photosystem I and the limitations imposed by the finite time resolution in single photon counting experiments. In particular, we show that rising components, associated with excitation transfer among different spectral forms, with lifetimes <20 ps would be undetected in a typical photon counting experiment.

journal_name

Biophys J

journal_title

Biophysical journal

authors

Jean JM,Chan CK,Fleming GR,Owens TG

doi

10.1016/S0006-3495(89)82767-5

subject

Has Abstract

pub_date

1989-12-01 00:00:00

pages

1203-15

issue

6

eissn

0006-3495

issn

1542-0086

pii

S0006-3495(89)82767-5

journal_volume

56

pub_type

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