Field-free molecular alignment induced by elliptically polarized laser pulses: non invasive 3 dimensional characterization

TL;DR

This paper demonstrates a non-invasive optical method to characterize 3D molecular alignment in CO₂ induced by elliptically polarized laser pulses, revealing effects similar to superposition of two cross-polarized pulses and highlighting a 'magic angle' analogy.

Contribution

It introduces an all-optical, non-invasive technique for 3D molecular alignment measurement and compares experimental results with theoretical predictions, emphasizing the effects of ellipticity.

Findings

Alignment amplitude and shape match theoretical models.

Elliptical polarization induces near-superposition of effects from two cross-polarized pulses.

Field-free two-direction alignment alternation occurs at specific ellipticities.

Abstract

An investigation of field-free molecular alignment produced by elliptically polarized laser pulses is reported. Experiments are conducted in CO$_2$ at room temperature. A non invasive all-optical technique, based on the cross defocusing of a probe pulse, is used to measure the alignment along two orthogonal directions that is sufficient to provide a 3 dimensional characterization. The field-free molecular alignment produced by a laser of elliptical polarization is in good agreement in terms of amplitude and shape with theoretical predictions. It turns out to be almost equivalent to the superposition of the effects that one would obtain with two individual cross-polarized pulses. The investigation highlights notably the occurrence of field-free two-direction alignment alternation for a suitably chosen degree of ellipticity. The analogy between this specific ellipticity and the well known "magic angle" used in time resolved spectroscopy to prevent rotational contributions is discussed.