Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 23, Pages 5878-5883Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b02754
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Funding
- Fonds National Suisse de la Recherche Scientifique [200020-165890]
- University of Geneva
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Most quadrupolar molecules designed for large two-photon absorption cross section have been shown to undergo symmetry breaking upon excitation to the S-1 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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