Circular dichroism in molecular frame photoemission Academic Article uri icon

abstract

  • The paper reports on a comparative experimental and theoretical study of circular dichroism in electron angular distribution (CDAD) in the molecular frame (MF) of linear molecules photoionized by circularly or elliptically polarized light. The CDAD is derived from the analysis of the complete molecular frame angular distribution (MFPAD) I(,e,e), where is the orientation of the molecule with respect to the light propagation axis and (e,e) the electron emission direction in the MF, using the vector correlation method. The CDAD is quantified by the e dependence of the left-right emission asymmetry maximum in the plane perpendicular to the light propagation axis k, for a space fixed molecule orthogonal to k. The experimental results for selected valence shell photoionization (PI) reactions in NO, O2, N2O compare very well with the multichannel Schwinger configuration interaction (MCSCI) ab initio calculations. Combined with a simple model of the ionization process, including the partial-wave composition of the initial state and phase shifts estimated from quantum defects for the various scattering partial-waves, these results provide the basis for a general discussion of the circular dichroism effect. This study enables one to disentangle the influence of the (sp, p) initial valence shell ionized orbital and that of the scattering dynamics on some fingerprint properties of the CDAD. On the other hand, the CDAD for s K-shell is purely assigned to a final state scattering effect. This analysis will be extended to PI of non-linear molecules where the circular dichroism characterizes recoil frame photoelectron angular distributions (RFPADs).

published proceedings

  • Molecular Physics

author list (cited authors)

  • Dowek, D., Lebech, M., Houver, J. C., & Lucchese, R. R.

citation count

  • 14

complete list of authors

  • Dowek, D||Lebech, M||Houver, JC||Lucchese, RR

publication date

  • June 2007