Anomalous Temperature Dependence of Exciton Spectral
Diffusion in Tetracene Thin Film
Posted on 2020-06-18 - 16:35
In this work, an ultrafast spectral
diffusion of the lowest exciton
in a tetracene ultrathin film is studied by two-dimensional electronic
spectroscopy. From the analysis of the nodal line slope, the frequency-fluctuation
correlation function (FFCF) of the exciton band is extracted. The
FFCF contains two components with decay times of 400 and 80 fs; while
the former can be understood by a linear exciton–phonon coupling
model, the latter shows an order of magnitude increase in its amplitude
from 96 to 186 K that cannot be explained by the same model. A novel
scheme of the energy-gap fluctuations is examined, in which an intramolecular
high-frequency mode causes the spectral diffusion that is enhanced
through an anharmonic coupling to low-frequency phonon modes. This
finding provides a valuable input for future theoretical predictions
on the ultrafast nonadiabatic dynamics of the molecular exciton.
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Yoshida, Tatsuya; Watanabe, Kazuya; Petrović, Marin; Kralj, Marko (2020). Anomalous Temperature Dependence of Exciton Spectral
Diffusion in Tetracene Thin Film. ACS Publications. Collection. https://doi.org/10.1021/acs.jpclett.0c01537
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AUTHORS (4)
TY
Tatsuya Yoshida
KW
Kazuya Watanabe
MP
Marin Petrović
MK
Marko Kralj