A quadrupolar A-𝜋-D-𝜋-A molecular rod with strong vibrational markers localized in the 𝜋-bridges and the A groups was used to investigate the symmetry breaking of the electronic distribution upon photoexcitation. Transient infrared spectroscopy allows the charge flow to be monitored on a femto-picosecond timescale with a submolecular spatial resolution. The infrared spectra of the molecule in the S1 state exhibit a remarkable solvent dependence (compare cyclohexane CHX with acetonitrile ACN). The symmetry-breaking process is entirely governed by the solvent; i.e. by the amplitude and fluctuations of the solvent field. Understanding the charge (de)localization and dynamics in the S1 state is of paramount importance for numerous possible applications of these strong two-photon absorbers.
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