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

Abstract

We present a theoretical study of recent laser-alignment and mixed-field-orientation experiments of asymmetric top molecules. In these experiments, pendular states were created using linearly polarized strong ac electric fields from pulsed lasers in combination with weak electrostatic fields. We compare the outcome of our calculations with experimental results obtained 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 directional properties of the molecular ensemble for several field configurations, i.e., for various field strengths and angles between ac and dc fields. For perpendicular fields one obtains pure alignment, which is well reproduced by the simulations. For tilted fields, we show that a fully adiabatic description of the process does not reproduce the experimentally observed orientation, and it is mandatory to use a diabatic model for population transfer between rotational states. We develop such a model and compare its outcome to the experimental data confirming the importance of non-adiabatic processes in the field-dressed molecular dynamics.

11 pages, 9 figures

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• Non-adiabatic effects in long-pulse mixed-field orientation of a linear polar molecule
• Time-dependent analysis of the mixed-field orientation of molecules without rotational symmetry
• Rotational spectrum of asymmetric top molecules in combined static and laser fields
• Rotational dynamics of an asymmetric top molecule in parallel electric and non-resonant laser fields
• Theoretical description of mixed-field orientation of asymmetric top molecules: a time-dependent study
• Orientation and Alignment Dynamics of Polar Molecule Driven by Shaped Laser Pulses
• Theoretical study of asymmetric superrotors: alignment and orientation
• Analyzing laser-induced alignment of weakly-bound molecular aggregates
• Laser-induced molecular alignment in the presence of chaotic rotational dynamics
• Mixed-field orientation of a thermal ensemble of linear polar molecules