Single and multi-photon ionization of aligned molecular ensembles is examined, with a particular focus on the link between the molecular axis distribution and observable in various angle-integrated and angle-resolved measurements. To maintain generality the problem is treated geometrically, with the aligned ensemble cast in terms of axis distribution moments, and the response of observables in terms of couplings to these moments. Within this formalism the angular momentum coupling is treated analytically, allowing for general characteristics - independent of the details of the ionization dynamics of a specific molecule - to be determined. Limiting cases are explored in order to provide a phenomenology which should be readily applicable to a range of experimental measurements, and illustrate how observables can be sensitive to fine details of the alignment, i.e. higher-order moments of the axis distribution, which are often neglected in experimental studies. We hope that this detailed and comprehensive treatment will bridge the gap between existing theoretical and experimental works, and provide both quantitative physical insights and a useful general phenomenology for researchers working with aligned molecular ensembles.
New Journal of Physics17, 23069 (24 February 2015).