ArticleNature chemistry2025
Vibronic coupling-driven symmetry breaking and solvation in the photoexcited dynamics of quadrupolar dyes.
Article in Nature chemistry, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 9 papers.
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Who cites it
9 citing papers in PubMed.
- Functional matrix engineering enables aggregate-state photophysics in tumor-responsive organic NIR-II phototheranostics.Materials today. Bio · 2026Article
- Excited-state conformational flexibility enables intrinsic amplification of circularly polarized luminescence.Chemical science · 2026Article
- Solvent Polarity as a Diagnostic for Vibronic/Vibrational Coherences Distinction in an Efficient TADF-TTA Switchable Emitter.Small science · 2026Article
- Article
- Direct Observation of Franck-Condon Stimulated Emission and Sub-20 fs Relaxation in Photoexcited Flavins.The journal of physical chemistry letters · 2026Article
- Molecular Origin of Correlated Bath Effects in Photoinduced Charge Transfer Dynamics in Polar Solvents.The journal of physical chemistry letters · 2026Article
- Signatures of Antisymmetric Vibrations in the Ultrafast Dynamics of Quadrupolar Dyes.The journal of physical chemistry letters · 2026Article
- Consistent and Generalizable Effective Model Hamiltonian Framework for Studying Nonadiabatic Dynamics in the Condensed Phase.Journal of chemical theory and computation · 2025Review
- Vibronic coupling-driven symmetry breaking and solvation in the photoexcited dynamics of quadrupolar dyes.Nature chemistry · 2025Article
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Authors and funding
12 authors.
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Abstract
Quadrupolar dyes, such as acceptor-donor-acceptor molecules, are highly relevant for applications in nonlinear optics and photovoltaics. They are also versatile models for exploring photoinduced charge-transfer dynamics. The interplay between electronic and vibronic couplings in these molecules may break excited-state symmetry, resulting in intramolecular charge separation and pronounced solvatochromism. Experimentally, distinguishing the roles of intramolecular vibronic coupling and solvent reorganization for the initial charge-transfer dynamics has been challenging so far. Here we investigate a prototypical quadrupolar dye in polar and non-polar solvents using ultrafast pump-probe and two-dimensional electronic spectroscopy. Our results reveal that vibronic couplings initiate excited-state symmetry breaking during the first ~50 fs of the photoinduced charge transfer, whereas solvent-induced charge localization sets in at later times. Quantum dynamics and electronic structure simulations support our experimental findings. Our results reveal the details of solvation dynamics in photoexcited molecules and suggest strategies for their manipulation through vibronic couplings.
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