Kim, J., Nguyen-Phan, T. C., Gardiner, A. T., Yoon, T. H., Cogdell, R. J. , Cho, M. and Scholes, G. D. (2022) Vibrational modes promoting exciton relaxation in the B850 band of LH2. Journal of Physical Chemistry Letters, 13(4), pp. 1099-1106. (doi: 10.1021/acs.jpclett.1c03868) (PMID:35080414)
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Abstract
Exciton relaxation dynamics in multichromophore systems are often modeled using Redfield theory, where bath fluctuations mediate the relaxation among the exciton eigenstates. Identifying the vibrational or phonon modes that are implicated in exciton relaxation allows more detailed understanding of exciton dynamics. Here we focus on a well-studied light-harvesting II complex (LH2) isolated from the photosynthetic purple bacterium Rhodoblastus acidophilus strain 10050. Using two synchronized mode-locked lasers, we carried out a polarization-dependent two-dimensional electronic spectroscopy (2DES) study of an ultrafast exciton relaxation in the B850 band of LH2. 2DES data with different polarization configurations enable us to investigate the exciton relaxation between the k = ±1 exciton states. Then, we identify vibrational modes coupled to the exciton relaxation by analyzing the coherent wavepackets in the 2DES signals. Focusing on the coherent vibrational wavepackets, the data suggest that certain symmetry-breaking modes of monomeric units play a key role in exciton relaxation.
| Item Type: | Articles |
|---|---|
| Additional Information: | This material is based upon work supported by the U.S. Department of Energy, Office of Basic Energy Sciences under contract DE-SC0020437 (J.K. and G.D.S.) and the Institute for Basic Science in Korea (IBS-R23-D1, T.H.Y. and M.C.). T.C.N. and R.J.C. were supported by BBSRC grant n. BB/ N0166734/1. A.T.G. and R.J.C. gratefully acknowledge funding from the Photosynthetic Antenna Research Center, an Energy Research Center funded by the Department of Energy, Office of Basic Energy Sciences, under award no. DESC0001035. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Cogdell, Professor Richard and Gardiner, Dr Alastair and Nguyen Phan, Cam Tu |
| Authors: | Kim, J., Nguyen-Phan, T. C., Gardiner, A. T., Yoon, T. H., Cogdell, R. J., Cho, M., and Scholes, G. D. |
| College/School: | College of Medical Veterinary and Life Sciences > School of Infection & Immunity College of Medical Veterinary and Life Sciences > School of Molecular Biosciences |
| Journal Name: | Journal of Physical Chemistry Letters |
| Publisher: | American Chemical Society |
| ISSN: | 1948-7185 |
| ISSN (Online): | 1948-7185 |
| Published Online: | 26 January 2022 |
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