Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

Björn Kriete, Julian Lüttig, Tenzin Kunsel, Pavel Malý, Thomas L. C. Jansen, Jasper Knoester, Tobias Brixner and Maxim S. Pshenichnikov ()
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Björn Kriete: University of Groningen, Zernike Institute for Advanced Materials
Julian Lüttig: Universität Würzburg, Am Hubland
Tenzin Kunsel: University of Groningen, Zernike Institute for Advanced Materials
Pavel Malý: Universität Würzburg, Am Hubland
Thomas L. C. Jansen: University of Groningen, Zernike Institute for Advanced Materials
Jasper Knoester: University of Groningen, Zernike Institute for Advanced Materials
Tobias Brixner: Universität Würzburg, Am Hubland
Maxim S. Pshenichnikov: University of Groningen, Zernike Institute for Advanced Materials

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Unraveling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a combination of delocalized excitation wavefunctions (excitons) and exciton diffusion. The unambiguous identification of the exciton transport is intrinsically challenging due to the system’s sheer complexity. Here we address this challenge by employing a spectroscopic lab-on-a-chip approach: ultrafast coherent two-dimensional spectroscopy and microfluidics working in tandem with theoretical modeling. We show that at low excitation fluences, the outer layer acts as an exciton antenna supplying excitons to the inner tube, while under high excitation fluences the former converts its functionality into an exciton annihilator which depletes the exciton population prior to any exciton transfer. Our findings shed light on the excitonic trajectories across different sub-units of a multi-layered artificial light-harvesting complex and underpin their great potential for directional excitation energy transport.

Date: 2019
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DOI: 10.1038/s41467-019-12345-9

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