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

Dereka, Bogdan; Rosspeintner, Arnulf; Stężycki, Rafał; Ruckebusch, Cyril; Gryko, Daniel T.; Vauthey, Eric

doi:10.1021/acs.jpclett.7b02944

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Title		Excited-State Symmetry Breaking in a Quadrupolar Molecule Visualized in Time and Space
Authors		Dereka, Bogdan Rosspeintner, Arnulf Stężycki, Rafał Ruckebusch, Cyril Gryko, Daniel T. Vauthey, Eric
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.
Identifiers		DOI: 10.1021/acs.jpclett.7b02944
Full text		Article (Published version) (1.8 MB) - Limited access to UNIGE Other version: https://pubs.acs.org/doi/10.1021/acs.jpclett.7b02944
Structures		Faculté des sciences / Section de chimie et biochimie / Département de chimie physique
Citation (ISO format)		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