Abstract
For a model of the B850 band in the light harvesting complex 2 of purple bacteria, the main quantum mechanical characteristics of the single complex line shapes are studied based on the theory of the preceding paper. The model consists of single exciton states coupled to harmonic oscillator bath, with the inclusion of both static and quasistatic disorder within the exciton Hamiltonian. A closed form line shape expression is derived that can account for the non-Markovian nature of the bath for a general spectral density. The calculation of the line shape only requires the inversion of a small matrix with dimension equal to the number of exciton levels, at each frequency. For two examples of site energy modulation with definite symmetries, we examine the dependencies of the line shape on the polarization of the radiation, on the type of exciton–bath coupling, and on temperature. For a plausible example of disorder, we simulate the line shapes of the ensemble and single complex spectroscopies. Simulation of single complex line shapes suggests that the quasistatic disorder is responsible for large spectral jumps (spectral diffusion) of the lowest exciton state and make the widths of the two brightest peaks comparable.
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Dates
Type | When |
---|---|
Created | 22 years, 3 months ago (May 15, 2003, 7:33 p.m.) |
Deposited | 1 year, 6 months ago (Feb. 7, 2024, 8:08 a.m.) |
Indexed | 1 year ago (Aug. 12, 2024, 7:15 a.m.) |
Issued | 22 years, 3 months ago (May 22, 2003) |
Published | 22 years, 3 months ago (May 22, 2003) |
Published Print | 22 years, 3 months ago (May 22, 2003) |
@article{Jang_2003, title={Single complex line shapes of the B850 band of LH2}, volume={118}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.1569240}, DOI={10.1063/1.1569240}, number={20}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Jang, Seogjoo and Silbey, Robert J.}, year={2003}, month=may, pages={9324–9336} }