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.

] Department of Chemical Physics Lund University PO Box 124 SE 22100 Lund Sweden [2] Department of Chemical Physics Charles University Prague Ke Karlovu 3 121 16 Praha 2 Czech Republic

Departamento de Física Aplicada Universidad Politécnica de Cartagena Cartagena 30202 Spain

Department of Chemical Physics Lund University PO Box 124 SE 22100 Lund Sweden

Forschungszentrum für Elektronenmikroskopie Institut für Chemie und Biochemie Freie Universität Berlin Fabeckstraβe 36a D 14195 Berlin Germany

Institut für Theoretische Physik Universität Ulm Albert Einstein Allee 11 89069 Ulm Germany

Photonics Institute Vienna University of Technology Gusshausstrasse 27 1040 Vienna Austria

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