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Photoionization of randomly oriented chiral molecules with circularlypolarized light leads to a strong forward/backward asymmetry in thephotoelectron angular distribution. This chiroptical effect, referred to asPhotoelectron Circular Dichroism (PECD), was shown to take place in allionization regimes, from single photon to tunnel ionization. In the ResonanceEnhanced Multiphoton Ionisation (REMPI) regime, where most of the table-topPECD experiments have been performed, understanding the role of theintermediate resonances is currently the subject of experimental andtheoretical investigations. In an attempt to decouple the role of bound-boundand bound-continuum transitions in REMPI-PECD, we photoionized the (+)-limoneneenantiomer using two-color laser fields in [1+1'] and [2+2'] ionizationschemes, where the polarization state of each color can be controlledindependently. We demonstrate that the main effect of the bound-boundtransition is to break the sample isotropy by orientation-dependentphotoexcitation, in agreement with recent theoretical pre- dictions. We showthat the angular distribution of PECD strongly depends on the anisotropy ofphotoexcitation to the intermediate state, which is different for circularlyand linearly polarized laser pulses. On the contrary, the helicity of the pulsethat drives the bound-bound transition is shown to have a negligible effect onthe PECD.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Multiphoton Photoelectron Circular Dichroism of Limonene with  Independent Polarization State Control of the Bound-Bound and Bound-Continuum  Transitions