Non-adiabatic effects in long-pulse mixed-field orientation of a linear polar molecule

Abstract

We present a theoretical study of the impact of an electrostatic field combined with non-resonant linearly polarized laser pulses on the rotational dynamics of linear molecules. Within the rigid rotor approximation, we solve the time-dependent Schrödinger equation for several field configurations. Using the OCS molecule as prototype, the field-dressed dynamics is analyzed in detail for experimentally accessible static field strengths and laser pulses. Results for directional cosines are presented and compared to the predictions of the adiabatic theory. We demonstrate that for prototypical field configuration used in current mixed-field orientation experiments, the molecular field dynamics is, in general, non-adiabatic, being mandatory a time-dependent description of these systems. We investigate several field regimes identifying the sources of non-adiabatic effects, and provide the field parameters under which the adiabatic dynamics would be achieved.

16 pages, 16 figures. Submitted to Physical Review A

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• 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
• Fine Structure of Open Shell Diatomic Molecules in Combined Electric and Magnetic Fields
• Theoretical study of asymmetric superrotors: alignment and orientation
• Analyzing laser-induced alignment of weakly-bound molecular aggregates
• Mixed-field orientation of a thermal ensemble of linear polar molecules
• An introduction to classical monodromy: applications to molecules in external fields