研究目的
Investigating the transient glass formation around a quadrupolar photoexcited dye in a strongly H-bonding liquid observed by transient 2D-IR spectroscopy.
研究成果
Transient 2D-IR spectroscopy has provided unprecedented insight into H-bonding dynamics in an electronically excited state, revealing the subtle interplay between intramolecular charge transfer, hydrogen-bond interactions, and solvation. The study monitored solvent motion around an excited quadrupolar molecule at different stages during the formation of a tight asymmetric H-bonded complex, observing a dramatic stiffening of the environment upon complex-formation, leading to a glass-like behavior with no spectral diffusion observed on the typical timescale of solvent motion.
研究不足
The 2D-IR signal of ESA2 and 4, due to the CN group located on the other, less-polar side of ADA, is too weak and decays too rapidly to extract quantitative information. The study is limited to the timescale accessible in the 2D experiment, and the most tightly-bound complexes may be in equilibrium with the loosely-bound subpopulation on a significantly slower timescale.