Vibronic origin of long-lived coherence in an artificial molecular light harvester

James Lim, David Paleček, Felipe Caycedo-Soler, Craig N. Lincoln, Javier Prior, Hans von Berlepsch, Susana F. Huelga, Martin B. Plenio, Donatas Zigmantas and Jürgen Hauer ()
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James Lim: Institut für Theoretische Physik, Universität Ulm
David Paleček: Lund University
Felipe Caycedo-Soler: Institut für Theoretische Physik, Universität Ulm
Craig N. Lincoln: Photonics Institute, Vienna University of Technology
Javier Prior: Universidad Politécnica de Cartagena
Hans von Berlepsch: Forschungszentrum für Elektronenmikroskopie, Institut für Chemie und Biochemie, Freie Universität Berlin
Susana F. Huelga: Institut für Theoretische Physik, Universität Ulm
Martin B. Plenio: Institut für Theoretische Physik, Universität Ulm
Donatas Zigmantas: Lund University
Jürgen Hauer: Photonics Institute, Vienna University of Technology

Nature Communications, 2015, vol. 6, issue 1, 1-7

Abstract: Abstract Natural and artificial light-harvesting processes have recently gained new interest. Signatures of long-lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton–vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization-controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.

Date: 2015
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DOI: 10.1038/ncomms8755

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