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Excited-State Symmetry Breaking in a Quadrupolar Molecule Visualized in Time and Space

Stężycki, Rafał
Ruckebusch, Cyril
Gryko, Daniel T.
Published in The journal of physical chemistry letters. 2017, vol. 8, no. 24, p. 6029-6034
Abstract The influence of the length of the push–pull branches of quadrupolar molecules on their excited-state symmetry breaking was investigated using ultrafast time-resolved IR spectroscopy. For this, the excited-state dynamics of an A-π-D-π-A molecule was compared with those of an ADA analogue, where the same electron donor (D) and acceptor (A) subunits are directly linked without a phenylethynyl π-spacer. The spatial distribution of the excitation was visualized in real time by monitoring C≡C and C≡N vibrational modes localized in the spacer and acceptor units, respectively. In nonpolar solvents, the excited state is quadrupolar and the excitation is localized on the π-D-π center. In medium polarity solvents, the excitation spreads over the entire molecule but is no longer symmetric. Finally, in the most polar solvents, the excitation localizes on a single D-π-A branch, contrary to the ADA analogue where symmetry breaking is only partial.
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DEREKA, Bogdan et al. Excited-State Symmetry Breaking in a Quadrupolar Molecule Visualized in Time and Space. In: Journal of Physical Chemistry Letters, 2017, vol. 8, n° 24, p. 6029-6034. doi: 10.1021/acs.jpclett.7b02944 https://archive-ouverte.unige.ch/unige:140498

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Deposited on : 2020-08-31

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