Measurement of circular dichroism in rotationally resolved photoelectron angular distributions following the photoionization of NO A 2Σ+

Abstract
The photoionization process NO A 2Σ+ (v=0, N=22)→NO+ X 1Σ+ (v+=0, N+)+e is studied with sufficient photoelectron energy resolution that the photoelectron angular distributions (PADs) associated with individual rotational levels N+ of the ion are determined. By ionizing with left and right circularly polarized light and observing the change in the rotationally resolved PADs, we can deduce all dynamical information, including the signs of the relative phase shifts of the photoelectron partial waves. This information constitutes the first complete description of the photoionization of a molecule. We discuss the consistency of our dynamical parameters with the Rydberg series of NO. We present a general formalism for (1+1’) resonance‐enhanced multiphoton ionization (REMPI) PADs for rotationally resolved ion states using linearly polarized light for excitation and elliptically polarized light for ionization. Based on the dynamical parameters determined from our fit, we use this formalism to predict the total system state, i.e., three‐dimensional PADs and polarization of ion rotational levels following photoionization.

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