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• W2019464878 endingPage "4515" @default.
• W2019464878 startingPage "4500" @default.
• W2019464878 abstract "Ultrafast polarized pump–probe spectroscopy has been used to study the ICN Ã band photodissociation dynamics in several molecular liquids (water, ethanol, methanol, and chloroform). By exciting at 224 and 255 nm and probing at 385 nm near the gas phase CN B←X transition, the population and vector correlations in the resulting products have been followed with ∼150 fs time resolution. The exhaustive gas-phase reaction dynamics charted for this system indicate that a substantial torque is imparted to the CN fragment in the ground state I dissociation channel while the CN is rotationally cold in the I* channel. The fate of the highly rotationally excited fragment in a liquid environment is explored in the present study. The transient pump–probe anisotropy in ethanol and methanol shows two time scales for decay, ∼400 fs and 3–7 ps depending on excitation energy; the two time scales are assigned to the two product channels. The subpicosecond time scale is characteristic of rotational diffusion of thermalized CN while the longer several picosecond time scale suggests the rotationally hot CN rotate nearly freely for several picoseconds in the plane defined by the initial dissociative event. The rotational behavior of a diatomic fragment is considered between the free rotor and small-angle rotational diffusion limits. The CN photoproduct population dynamics are quite varied in the different solvents. In alcohols and chloroform, CN undergoes abstraction reactions with the solvent while in water there is no abstraction. Caging and diffusive geminate recombination dynamics apparently vary markedly in the different solvents; these effects are compared to molecular dynamics results for this photodissociation system. A large isotope effect is observed between H2O and D2O solvents in the product recombination dynamics." @default.
• W2019464878 created "2016-06-24" @default.
• W2019464878 creator A5013732819 @default.
• W2019464878 creator A5034301199 @default.
• W2019464878 date "2003-08-08" @default.
• W2019464878 modified "2023-09-23" @default.
• W2019464878 title "Photodissociation of ICN in polar solvents: Evidence for long lived rotational excitation in room temperature liquids" @default.
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