Abstract
Liquid and supercritical ammonia (NH3) is photo-ionized at an energy of 9.3 eV with 100-fs duration pulses at a wavelength of 266 nm. The ionization involves two photons and generates fully solvated electrons via the conduction band of the solvent within the time resolution of the experiment. The dynamics of their ensuing geminate recombination is followed in real time with femtosecond near-infrared (IR) probe pulses. The recombination mechanism can be understood as an ion-pair mediated reaction. The electron survival probability is found to be in quantitative agreement with the classical Onsager theory for the initial recombination of ions.
Highlights
Solvated electrons are the most fundamental spin centers in condensed phase chemistry and have raised considerable attention of the physical and theoretical chemistry communities
The electron survival probability is found to be in quantitative agreement with the classical Onsager theory for the initial recombination of ions
Solvation and thermal relaxation, or reactive and non-reactive electron-solvent scattering including charge transfer are all fundamental processes that contribute to the complex coupled electron-solvent dynamics that follow an initial injection of a single electronic spin center into the liquid
Summary
Solvated electrons are the most fundamental spin centers in condensed phase chemistry and have raised considerable attention of the physical and theoretical chemistry communities. The ionization involves two photons and generates fully solvated electrons via the conduction band of the solvent within the time resolution of the experiment. The dynamics of their ensuing geminate recombination is followed in real time with femtosecond near-infrared (IR) probe pulses.
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