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Evidence of excited state localization and static disorder in LH2 investigated by 2D-polarization single-molecule imaging at room temperature.

Tubasum, Sumera LU ; Camacho Dejay, Rafael LU ; Meyer, Matthias LU ; Yadav, Dheerendra LU ; Cogdell, Richard J ; Pullerits, Tönu LU and Scheblykin, Ivan LU (2013) In Physical Chemistry Chemical Physics 15(45). p.19862-19869
Abstract
Two-dimensional polarization fluorescence imaging of single light harvesting complexes 2 (LH2) of Rps. acidophila was carried out to investigate the polarization properties of excitation and fluorescence emission simultaneously, at room temperature. In two separate experiments we excited LH2 with a spectrally narrow laser line matched to the absorption bands of the two chromophore rings, B800 and B850, thereby indirectly and directly triggering fluorescence of the B850 exciton state. A correlation analysis of the polarization modulation depths in excitation and emission for a large number of single complexes was performed. Our results show, in comparison to B800, that the B850 ring is a more isotropic absorber due to the excitonic nature... (More)
Two-dimensional polarization fluorescence imaging of single light harvesting complexes 2 (LH2) of Rps. acidophila was carried out to investigate the polarization properties of excitation and fluorescence emission simultaneously, at room temperature. In two separate experiments we excited LH2 with a spectrally narrow laser line matched to the absorption bands of the two chromophore rings, B800 and B850, thereby indirectly and directly triggering fluorescence of the B850 exciton state. A correlation analysis of the polarization modulation depths in excitation and emission for a large number of single complexes was performed. Our results show, in comparison to B800, that the B850 ring is a more isotropic absorber due to the excitonic nature of its excited states. At the same time, we observed a strong tendency for LH2 to emit with dipolar character, from which preferential localization of the emissive exciton, stable for minutes, is inferred. We argue that the observed effects can consistently be explained by static energetic disorder and/or deformation of the complex, with possible involvement of exciton self-trapping. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
15
issue
45
pages
19862 - 19869
publisher
Royal Society of Chemistry
external identifiers
  • wos:000326470200042
  • pmid:24145962
  • scopus:84887002837
ISSN
1463-9084
DOI
10.1039/c3cp52127c
language
English
LU publication?
yes
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
id
9aae3a31-e1f4-4dda-9807-811e347719e9 (old id 4143126)
date added to LUP
2016-04-01 10:47:09
date last changed
2020-05-06 01:54:11
@article{9aae3a31-e1f4-4dda-9807-811e347719e9,
  abstract     = {Two-dimensional polarization fluorescence imaging of single light harvesting complexes 2 (LH2) of Rps. acidophila was carried out to investigate the polarization properties of excitation and fluorescence emission simultaneously, at room temperature. In two separate experiments we excited LH2 with a spectrally narrow laser line matched to the absorption bands of the two chromophore rings, B800 and B850, thereby indirectly and directly triggering fluorescence of the B850 exciton state. A correlation analysis of the polarization modulation depths in excitation and emission for a large number of single complexes was performed. Our results show, in comparison to B800, that the B850 ring is a more isotropic absorber due to the excitonic nature of its excited states. At the same time, we observed a strong tendency for LH2 to emit with dipolar character, from which preferential localization of the emissive exciton, stable for minutes, is inferred. We argue that the observed effects can consistently be explained by static energetic disorder and/or deformation of the complex, with possible involvement of exciton self-trapping.},
  author       = {Tubasum, Sumera and Camacho Dejay, Rafael and Meyer, Matthias and Yadav, Dheerendra and Cogdell, Richard J and Pullerits, Tönu and Scheblykin, Ivan},
  issn         = {1463-9084},
  language     = {eng},
  number       = {45},
  pages        = {19862--19869},
  publisher    = {Royal Society of Chemistry},
  series       = {Physical Chemistry Chemical Physics},
  title        = {Evidence of excited state localization and static disorder in LH2 investigated by 2D-polarization single-molecule imaging at room temperature.},
  url          = {http://dx.doi.org/10.1039/c3cp52127c},
  doi          = {10.1039/c3cp52127c},
  volume       = {15},
  year         = {2013},
}