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Title: Fluorescence Spectroscopy, Exciton Dynamics and Photochemistry of Single Allophycocyanin Trimers

Journal Article · · Journal of Physical Chemistry B
DOI:https://doi.org/10.1021/jp983227d· OSTI ID:15001947
 [1];  [2]
  1. ASSOC WESTERN UNIVERSITY
  2. HARVARD UNIVERSITY

We report a study of the spectroscopy and exciton dynamics of the allophycocyanin trimer (APC), a light harvesting protein complex from cyanobacteria, by room-temperature single-molecule measurements of fluorescence spectra, lifetimes, intensity trajectories and polarization modulation. Emission spectra of individual APC trimers are found to be homogeneous on the time scale of seconds. In contrast, their emission lifetimes are found to be widely distributed, because of generation of exciton traps during the course of measurements. The intensity trajectories and polarization modulation experiments indicate reversible ixciton trap formation within the three quasi-independent pairs of strong interacting a84 and B84 chromophores in APC, as well a photobleaching of individual chromophores. Comparison experiments under continuous wave and pulsed excitation reveal a two-photon mechanism for generating exciton traps and/or photobleaching, which involves exciton-exciton annihilation. These single-molecule experiments provide new insights into exciton dynamics and photochemistry of light-harvesting complexes.

Research Organization:
Pacific Northwest National Lab., Richland, WA (US)
Sponsoring Organization:
US Department of Energy (US)
DOE Contract Number:
AC06-76RL01830
OSTI ID:
15001947
Report Number(s):
PNNL-SA-30274; KC0301020; TRN: US0400537
Journal Information:
Journal of Physical Chemistry B, Vol. 102, Issue 50; Other Information: PBD: 1 Jan 1998
Country of Publication:
United States
Language:
English