Accessing the molecular frame through strong-field alignment of distributions of gas phase molecules

A rationale for creating highly aligned distributions of molecules is that it enables vector properties referenced to molecule-fixed axes (the molecular frame) to be determined. In the present work, the degree of alignment that is necessary for this to be achieved in practice is explored. Alignment is commonly parametrized in experiments by a single parameter, [Formula: see text], which is insufficient to enable predictive calculations to be performed. Here, it is shown that, if the full distribution of molecular axes takes a Gaussian form, this single parameter can be used to determine the complete set of alignment moments needed to characterize the distribution. In order to demonstrate the degree of alignment that is required to approach the molecular frame, the alignment moments corresponding to a few chosen values of [Formula: see text] are used to project a model molecular frame photoelectron angular distribution into the laboratory frame. These calculations show that [Formula: see text] needs to approach 0.9 in order to avoid significant blurring to be caused by averaging.This article is part of the theme issue 'Modern theoretical chemistry'.