Two-photon photochemistry: Angular distribution of photofragments and application to isotope separation

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Abstract
The resonant two‐photon dissociation process in a supersonic molecular beam is investigated. Angular distributions of photofragments in such a process are derived via a density matrix formalism. Conservation of angular momentum and bound‐continuum Franck–Condon factors determine the angular distributions and the photodissociation cross sections. Criteria which the polarization state of the photon fields and the initial J state of the molecule should meet, to have the largest cross section and good photofragment collection efficiency, are discussed. Applications are foreseen in laser isotope separation.