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Superradiance and Exciton Delocalization in Bacterial Photosynthetic Light-Harvesting Systems
Open accessAbstract
We present temperature-dependent fluorescence quantum yield and lifetime measurements on the LH-1 and LH-2 complexes of Rhodobacter sphaeroides and on the isolated B820 subunit of Rhodospirillum rubrum . From these measurements the superradiance is calculated, which is related to the delocalization of excitations in these complexes. In the B820 preparation we find a radiative rate that is 30% higher than that of monomeric bacteriochlorophyll, in agreement with a dimer model of this subunit. At room temperature both LH-1 and LH-2 are superradiant relative to monomeric Bchl- a with enhancement factors of 3.8 and 2.8, respectively. In LH-2 the radiative rate does not change significantly upon lowering the temperature to 4 K. LH-1 however exhibits a strong temperature dependence, giving rise to a 2.4 times higher radiative rate at 4 K relative to room temperature. From modeling of the superradiance using a Hamiltonian based on the LH-2 structure and including site inhomogeneity, we conclude that the ratio of inhomogeneity over the coupling between the pigments is around 1 for LH-1 and 2−3 for LH-2. From the Monte Carlo simulations we estimate the delocalization length in LH-1 and LH-2 to be on the order of 3−4 pigments at room temperature.
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Metadata
- Authors
- Monshouwer, R., Abrahamsson, M., van Mourik, F., & van Grondelle, R.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 1997-09-01
- Volume
- 101
- Issue
- 37
- Pages
- 7241-7248
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2171860962
- Cited by
- 406
- References
- 0
- FWCI
- 17.30
- Type
- journal article
- Language
- en
- Open access
- green
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- Monshouwer, R., Abrahamsson, M., van Mourik, F., & van Grondelle, R. (1997). Superradiance and Exciton Delocalization in Bacterial Photosynthetic Light-Harvesting Systems. The Journal of Physical Chemistry B. https://doi.org/10.1021/jp963377t
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