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We introduce a four-dimensional quantum model for describing the torsionalcontrol of $\rm G_{16}$-type molecules in the electronic ground state, based onthe symmetry-adapted variational method. We define conditions for whichlower-dimensional models, commonly used to simulate the strong-field control ofmolecular torsions, are reliable approximations to a four-dimensionaltreatment. In particular, we study the role of different types ofrotational-torsional couplings---the field-free coupling and the field-inducedcoupling---and show that the conclusions recently drawn on the role ofrotational-torsional couplings in the process of torsional alignment are notcorrect. Furthermore, we demonstrate how important an adequate description ofthe molecular polarizability is for reliably predicting the torsionalalignment.

A systematic four-dimensional approach to strong field control of molecular torsions