- 作者: Gunter Flachenecker and Arnulf Materny
- 中文摘要: We review recent work done on the femtosecond time-resolved investigation of the influence of solvation on elementary molecular and reaction dynamics of solvated molecules. Using the photo dissociation reaction of I2 and NaI molecules as models, the solvation effect is studied for varying environments. By adding inert gases (He, Ar, N2) at pressures ranging from 0 to 3000 bar, the dynamics is studied starting from isolated molecules, going steadily to solvent-like conditions. Clearly different reaction behaviour can be found when comparing I2 and NaI. While I2 molecules predissociate due to the collisions with the surrounding gas particles and afterwards recombine due to the caging effect, NaI is stabilized in its adiabatic potential well formed by the first excited electronic state and the ionic ground state. I2 is also embedded in a solid matrix, formed by a crystalline porosil. For I2 in both cases the recombination dynamics is studied by varying the probe wavelength. The experimental data are discussed using a theoretical model. For I2 in a high pressure gas environment, geminate primary and secondary recombination can be detected; in the porosils also nongeminate processes contribute on a very short time scale.
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