We introduce a four-dimensional quantum model for describing the torsional control of G16-type molecules in the electronic ground state, based on the symmetry-adapted variational method. We define conditions for which lower-dimensional models, commonly used to simulate the strong-field control of molecular torsions, are reliable approximations to a four-dimensional treatment. In particular, we study the role of different types of rotational-torsional couplings---the field-free coupling and the field-induced coupling---and show that the conclusions recently drawn on the role of rotational-torsional couplings in the process of torsional alignment are not correct. Furthermore, we demonstrate how important an adequate description of the molecular polarizability is for reliably predicting the torsional alignment.
@article{arxiv.1707.00022,
title = {A systematic four-dimensional approach to strong field control of molecular torsions},
author = {Thomas Grohmann and Monika Leibscher and Tamar Seideman},
journal= {arXiv preprint arXiv:1707.00022},
year = {2017}
}