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Thiessen A, Würsch D, Jester SS, et al. Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures. J Phys Chem B. 2015;119(30):9949-58doi: 10.1021/acs.jpcb.5b02091.
Thiessen, A., Würsch, D., Jester, S. S., Aggarwal, A. V., Idelson, A., Bange, S., Vogelsang, J., Höger, S., & Lupton, J. M. (2015). Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures. The journal of physical chemistry. B, 119(30), 9949-58. https://doi.org/10.1021/acs.jpcb.5b02091
Thiessen, Alexander, et al. "Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures." The journal of physical chemistry. B vol. 119,30 (2015): 9949-58. doi: https://doi.org/10.1021/acs.jpcb.5b02091
Thiessen A, Würsch D, Jester SS, Aggarwal AV, Idelson A, Bange S, Vogelsang J, Höger S, Lupton JM. Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures. J Phys Chem B. 2015 Jul 30;119(30):9949-58. doi: 10.1021/acs.jpcb.5b02091. Epub 2015 Jul 16. PMID: 26035080.
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J Phys Chem B. 2015 Jul 30;119(30):9949-58. doi: 10.1021/acs.jpcb.5b02091. Epub 2015 Jul 16.

Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures.

The journal of physical chemistry. B

Alexander Thiessen, Dominik Würsch, Stefan-S Jester, A Vikas Aggarwal, Alissa Idelson, Sebastian Bange, Jan Vogelsang, Sigurd Höger, John M Lupton

Affiliations

  1. †Department of Physics and Astronomy, University of Utah, Salt Lake City, Utah 84112, United States.
  2. ‡Institut für Experimentelle und Angewandte Physik, Universität Regensburg, 93040 Regensburg, Germany.
  3. §Kekulé-Institut für Organische Chemie und Biochemie der Universität Bonn, 53121 Bonn, Germany.

PMID: 26035080 DOI: 10.1021/acs.jpcb.5b02091

Abstract

We employ five π-conjugated model materials of different molecular shape-oligomers and cyclic structures-to investigate the extent of exciton self-trapping and torsional motion of the molecular framework following optical excitation. Our studies combine steady state and transient fluorescence spectroscopy in the ensemble with measurements of polarization anisotropy on single molecules, supported by Monte Carlo simulations. The dimer exhibits a significant spectral red shift within ∼100 ps after photoexcitation which is attributed to torsional relaxation. This relaxation mechanism is inhibited in the structurally rigid macrocyclic analogue. However, both systems show a high degree of exciton localization but with very different consequences: while, in the macrocycle, the exciton localizes randomly on different parts of the ring, scrambling polarization memory, in the dimer, localization leads to a deterministic exciton position with luminescence characteristics of a dipole. Monte Carlo simulations allow us to quantify the structural difference between the emitting and absorbing units of the π-conjugated system in terms of disorder parameters.

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