Two-photon state selection and angular momentum polarization probed by velocity map imaging: Application to H atom photofragment angular distributions from the photodissociation of two-photon state selected HCl and HBr

Manzhos, Sergei; Romanescu, Constantin; Loock, Hans-Peter and Underwood, Jonathan G. (2004). Two-photon state selection and angular momentum polarization probed by velocity map imaging: Application to H atom photofragment angular distributions from the photodissociation of two-photon state selected HCl and HBr. Journal of Chemical Physics, 121(23) pp. 11802–11809.

DOI: https://doi.org/10.1063/1.1809571

Abstract

A formalism for calculating the angular momentum polarization of an atom or a molecule following two-photon excitation of a J-selected state is presented. This formalism is used to interpret the H atom photofragment angular distributions from single-photon dissociation of two-photon rovibronically state selected HCl and HBr prepared via a Q-branch transition. By comparison of the angular distributions measured using the velocity map imaging technique with the theoretical model it is shown that single-photon dissociation of two-photon prepared states can be used for pathway identification, allowing for the identification of the virtual state symmetry in the two-photon absorption and/or the symmetry of the dissociative state. It is also shown that under conditions of excitation with circularly polarized light, or for excitation via non-Q-branch transitions with linearly polarized light the angular momentum polarization is independent of the dynamics of the two-photon transition and analytically computable.©2004 American Institute of Physics.

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