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Observation of Vibronic -Coupling -Mediated Energy Transfer in Light-Harvesting Nanotubes Stabilized in a Solid-State Matrix

Accepted version
Peer-reviewed

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Type

Article

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Authors

Cheminal, Alexandre  ORCID logo  https://orcid.org/0000-0001-9969-672X
Thomas, Tudor 
Richter, Johannes 

Abstract

Ultrafast vibrational spectroscopy is employed to obtain real-time structural information of energy transport in double-walled light harvesting nanotubes at room temperature, stabilized in a host matrix to mimic the rigid scaffolds of natural light harvesting systems. We observe evidence of a low-frequency vibrational mode at 315 cm-1 which transfers excitons from the outer wall of the nanotubes to a crossing point through which energy transfer to the inner wall can occur. This mode is furthermore absent in solution phase. Importantly, the coherence of this mode is not transferred to the inner wall upon energy transfer and is only present on the outer wall’s excited state energy surface, highlighting that complete energy transfer between the outer and inner walls does not take place. Isolation of the individual walls of the nanotubes provides evidence that this mode corresponds to a supramolecular motion of the nanotubes. Our results emphasize the importance of the solid state environment in modulating vibronic coupling and directing energy transfer in molecular light-harvesting systems.

Description

Keywords

0306 Physical Chemistry (incl. Structural)

Journal Title

Journal of Physical Chemistry Letters

Conference Name

Journal ISSN

1948-7185
1948-7185

Volume Title

9

Publisher

American Chemical Society (ACS)
Sponsorship
Engineering and Physical Sciences Research Council (EP/M006360/1)
Engineering and Physical Sciences Research Council (EP/P027741/1)
EPSRC (1805376)
Winton Program for Physics of Sustainability
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