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Title

Specific Monitoring of Excited-State Symmetry Breaking by Femtosecond Broadband Fluorescence Upconversion Spectroscopy

Authors
Beckwith, Joseph S.
Lunzer, Markus
Holzer, Brigitte
Fröhlich, Johannes
Published in Journal of Physical Chemistry Letters. 2017, vol. 8, no. 23, p. 5878-5883
Abstract Most quadrupolar molecules designed for large two-photon absorption cross section have been shown to undergo symmetry breaking upon excitation to the S1 state. This was originally deduced from their strong fluorescence solvatochromism and later visualized in real time using transient infrared spectroscopy. For molecules not containing clear IR marker modes, however, a specific real-time observation of the symmetry breaking process remains lacking. Here we show that this process can be resolved using broadband fluorescence upconversion spectroscopy by monitoring the instantaneous emission transition dipole moment. This approach is illustrated with measurements performed on two quadrupolar molecules, with only one of them undergoing excited-state symmetry breaking in polar solvents.
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Other version: http://pubs.acs.org/doi/10.1021/acs.jpclett.7b02754
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Research group Groupe Vauthey
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BECKWITH, Joseph S. et al. Specific Monitoring of Excited-State Symmetry Breaking by Femtosecond Broadband Fluorescence Upconversion Spectroscopy. In: Journal of Physical Chemistry Letters, 2017, vol. 8, n° 23, p. 5878-5883. https://archive-ouverte.unige.ch/unige:100151

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Deposited on : 2017-12-12

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