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The transition between two distinct mechanisms for the laser-induced field-free orientation of CO molecules is observed via measurements of orientation revival times and subsequent comparison to theoretical calculations. In the first mechanism, which we find responsible for the orientation of CO up to peak intensities of 8 x 10^13 W/cm^2, the molecules are impulsively oriented through the hyperpolarizability interaction. At higher intensities, asymmetric depletion through orientation-selective ionization is the dominant orienting mechanism. In addition to the clear identification of the two regimes of orientation, we propose that careful measurements of the onset of the orientation depletion mechanism as a function of the laser intensity will provide a relatively simple route to calibrate absolute rates of non-perturbative strong-field molecular ionization.
Genetic algorithms, as implemented in optimal control strategies, are currently successfully exploited in a wide range of problems in molecular physics. In this context, laser control of molecular alignment and orientation remains a very promising is
We report the first experimental observation of non-adiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion
We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbow-like features in th
Alignment and orientation of molecules by intense, ultrashort laser fields are crucial for a variety of applications in physics and chemistry. These include control of high harmonics generation, molecular orbitals tomography, control of molecular pho
The strong coupling between intense laser fields and valence electrons in molecules causes a distortion of the potential energy hypersurfaces which determine the motion of nuclei in a molecule and influences possible reaction pathways. The coupling s