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Coupling to Charge Transfer States is the Key to Modulate the Optical Bands for Efficient Light Harvesting in Purple Bacteria

Cupellini, Lorenzo; Caprasecca, Stefano; Guido, Ciro A.; Müh, Frank; Renger, Thomas and Mennucci, Benedetta (2018). Coupling to Charge Transfer States is the Key to Modulate the Optical Bands for Efficient Light Harvesting in Purple Bacteria. The Journal of Physical Chemistry Letters, 9(23) pp. 6892–6899.

DOI (Digital Object Identifier) Link: https://doi.org/10.1021/acs.jpclett.8b03233
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Abstract

The photosynthetic apparatus of purple bacteria uses exciton delocalization and static disorder to modulate the position and broadening of its absorption bands, leading to efficient light harvesting. Its main antenna complex, LH2, contains two rings of identical bacteriochlorophyll pigments, B800 and B850, absorbing at 800 and 850 nm, respectively. It has been an unsolved problem why static disorder of the strongly coupled B850 ring is several times larger than that of the B800 ring. Here we show that mixing between excitons and charge transfer states in the B850 ring is responsible for the effect. The linear absorption spectrum of the LH2 system is simulated by using a multiscale approach with an exciton Hamiltonian generalized to include the charge transfer states that involve adjacent pigment pairs, with static disorder modeled microscopically by molecular dynamics simulations. Our results show that sufficient inhomogeneous broadening of the B850 band, needed for efficient light harvesting, is only obtained by utilizing static disorder in the coupling between local excited and interpigment charge transfer states.

Item Type: Journal Item
ISSN: 1948-7185
Academic Unit/School: Faculty of Science, Technology, Engineering and Mathematics (STEM) > Physical Sciences
Faculty of Science, Technology, Engineering and Mathematics (STEM)
Item ID: 58474
Depositing User: ORO Import
Date Deposited: 02 Jan 2019 09:37
Last Modified: 29 Mar 2019 10:36
URI: http://oro.open.ac.uk/id/eprint/58474
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