The mechanism of aggregation‐induced emission, which overcomes the common aggregation‐caused quenching problem in organic optoelectronics, is revealed by monitoring the real time structural evolution and dynamics of electronic excited state with frequency and polarization resolved ultrafast UV/IR spectroscopy and theoretical calculations. The formation of Woodward–Hoffmann cyclic intermediates upon ultraviolet excitation is observed in dilute solutions of tetraphenylethylene and its derivatives but not in their respective solid. The ultrafast cyclization provides an efficient nonradiative relaxation pathway through crossing a conical intersection. Without such a reaction mechanism, the electronic excitation is preserved in the molecular solids and the molecule fluoresces efficiently, aided by the very slow intermolecular charge and energy transfers due to the well separated molecular packing arrangement. The mechanisms can be general for tuning the properties of chromophores in different phases for various important applications.
Two-dimensional (2D) material-controllable degradation under light radiation is crucial for their photonics and medical-related applications, which are yet to be investigated. In this paper, we first report the laser illumination method to regulate the degradation rate of Ti3C2Tx nanosheets in aqueous solution. Comprehensive characterization of intermediates and final products confirmed that plasmonic laser promoting the oxidation was strikingly different from heating the aqueous solution homogeneously. Laser illumination would nearly 10 times accelerate the degradation of Ti3C2Tx nanosheets in initial stage and create many smaller-sized oxidized products in a short time.Laser-induced fast degradation was principally ascribed to surface plasmonic resonance effect of Ti3C2Tx nanosheets.The degradation ability of such illumination could be controlled either by tuning the excitation wavelength or changing the excitation power. Furthermore, the laser-or thermal-induced degradation could be retarded by surface protection of Ti3C2Tx nanosheets. Our results suggest that plasmonic electron excitation of Ti3C2Tx nanosheets could build a new reaction channel and lead to the fast oxidation of nanosheets in aqueous solution, potentially enabling a series of waterbased applications.
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