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We present a theoretical study of recent laser-alignment andmixed-field-orientation experiments of asymmetric top molecules. In theseexperiments, pendular states were created using linearly polarized strong acelectric fields from pulsed lasers in combination with weak electrostaticfields. We compare the outcome of our calculations with experimental resultsobtained for the prototypical large molecule benzonitrile (C$_7$H$_5$N) [J.L.Hansen et al, Phys. Rev. A, 83, 023406 (2011)] and explore the directionalproperties of the molecular ensemble for several field configurations, i.e.,for various field strengths and angles between ac and dc fields. Forperpendicular fields one obtains pure alignment, which is well reproduced bythe simulations. For tilted fields, we show that a fully adiabatic descriptionof the process does not reproduce the experimentally observed orientation, andit is mandatory to use a diabatic model for population transfer betweenrotational states. We develop such a model and compare its outcome to theexperimental data confirming the importance of non-adiabatic processes in thefield-dressed molecular dynamics.

Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model