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

The Journal of Physical Chemistry Letters
Raj PandyaAkshay Rao

Abstract

Ultrafast vibrational spectroscopy is employed to obtain real-time structural information on 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.

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Citations

Apr 30, 2020·Physical Chemistry Chemical Physics : PCCP·Björn KrieteMaxim S Pshenichnikov
Oct 12, 2019·Nature Communications·Björn KrieteMaxim S Pshenichnikov
Jan 20, 2021·Journal of the American Chemical Society·Jonathan D SchultzMichael R Wasielewski
Nov 16, 2019·The Journal of Physical Chemistry Letters·Jonathan D SchultzMichael R Wasielewski
Sep 29, 2020·Journal of the American Chemical Society·Björn KrieteMaxim S Pshenichnikov
Dec 1, 2020·The Journal of Physical Chemistry. a·Nadine C BradburyDaniel Neuhauser

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