Structural disorder within self-assembled molecular aggregates may have strong effects on their optical functionality. Such disorder, however, is hard to explore using standard ensemble measurements. In this paper, we report on the characterization of intra-aggregate structural disorder through a linewidth analysis of fluorescence excitation experiments on individual zinc-chlorin (ZnChl) nanotubular molecular aggregates. Recent experiments suggest an anomaly in the linewidths of the two absorption bands that dominate the spectra: the higher-energy bands on average show a smaller linewidth than the lower-energy bands. This anomaly is explored in this paper by analyzing and modeling the correlation of the two linewidths for each aggregate. We exploit a Frenkel exciton model to show that the experimentally observed correlation of linewidths and other statistical properties of the single-aggregate spectra can be explained from small variations of the molecular orientations within individual aggregates.
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Unraveling intra-aggregate structural disorder using single-molecule spectroscopy
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7 October 2020
Research Article|
October 05 2020
Unraveling intra-aggregate structural disorder using single-molecule spectroscopy
T. Kunsel
;
T. Kunsel
1
University of Groningen, Zernike Institute for Advanced Materials
, Nijenborgh 4, 9747 AG Groningen, The Netherlands
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A. Löhner
;
A. Löhner
2
Spectroscopy of Soft Matter, University of Bayreuth
, Universitätsstraße 30, 94557 Bayreuth, Germany
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J. J. Mayo;
J. J. Mayo
1
University of Groningen, Zernike Institute for Advanced Materials
, Nijenborgh 4, 9747 AG Groningen, The Netherlands
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J. Köhler
;
J. Köhler
2
Spectroscopy of Soft Matter, University of Bayreuth
, Universitätsstraße 30, 94557 Bayreuth, Germany
3
Bavarian Polymer Institute, University of Bayreuth
, Universitätsstraße 30, 94557 Bayreuth, Germany
4
Bayreuth Institute of Macromolecular Research (BIMF), University of Bayreuth
, Universitätsstraße 30, 94557 Bayreuth, Germany
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T. L. C. Jansen
;
T. L. C. Jansen
1
University of Groningen, Zernike Institute for Advanced Materials
, Nijenborgh 4, 9747 AG Groningen, The Netherlands
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J. Knoester
J. Knoester
a)
1
University of Groningen, Zernike Institute for Advanced Materials
, Nijenborgh 4, 9747 AG Groningen, The Netherlands
a)Author to whom correspondence should be addressed: j.knoester@rug.nl
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a)Author to whom correspondence should be addressed: j.knoester@rug.nl
Note: This paper is part of the JCP Special Topic on Excitons: Energetics and Spatio-Temporal Dynamics.
J. Chem. Phys. 153, 134304 (2020)
Article history
Received:
July 30 2020
Accepted:
September 14 2020
Citation
T. Kunsel, A. Löhner, J. J. Mayo, J. Köhler, T. L. C. Jansen, J. Knoester; Unraveling intra-aggregate structural disorder using single-molecule spectroscopy. J. Chem. Phys. 7 October 2020; 153 (13): 134304. https://doi.org/10.1063/5.0023551
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