Abstract
A multitude of possible applications along with unique coherence, chirality, and symmetry properties makes the control of molecular torsion with moderately strong, nonresonant laser pulses a fascinating subject. A description of combined rotation and torsion requires at least four angular degrees of freedom, which is challenging for the majority of systems. Lower-dimensional models have been proposed but also questioned. Here, we develop a four-dimensional model for the coupled rotational-torsional motions of molecules consisting of two identical moieties. By comparing four-dimensional calculations with a two-dimensional model, we define conditions under which the lower-dimensional model is valid. In particular, we point to the crucial role of coordinate dependence of the polarizability tensor. Our results do not agree with those of previous four-dimensional calculations but support the conclusions of recent experiments.
- Received 16 November 2016
DOI:https://doi.org/10.1103/PhysRevLett.118.203201
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