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Copyright Nature Publishing Group Jul 2015

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.

Details

Title
Vibronic origin of long-lived coherence in an artificial molecular light harvester
Author
Lim, James; Palecek, David; Caycedo-soler, Felipe; Lincoln, Craig N; Prior, Javier; Von Berlepsch, Hans; Huelga, Susana F; Plenio, Martin B; Zigmantas, Donatas; Hauer, Jürgen
Pages
7755
Publication year
2015
Publication date
Jul 2015
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
1695003269
Copyright
Copyright Nature Publishing Group Jul 2015