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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 photoionization and dissociation processes, production of molecular movies with the help of X-ray free-electron laser sources and ultrafast electron diffraction of relativistic electrons. While the dynamics of laser-induced molecular alignment has been extensively studied and demonstrated, molecular orientation is a much more challenging task, especially for asymmetric-top molecules. Here we report the first experimental demonstration of a field-free, all-optical three-dimensional orientation of asymmetric-top molecules by means of phase-locked cross-polarized two-color laser pulses. In addition to the conventional integrated orientation factor, we report the differential degree of orientation which is not amenable to optical measurements, but is readily accessible in our angle-resolved imaging technique. Our scheme applies to a wide class of asymmetric molecules and opens new ways towards controlling their orientation, eventually leading to direct imaging of structure of gas-phase molecules using advanced free electron laser beams with extremely high spatiotemporal resolution.
The yield of strong-field ionization, by a linearly polarized probe pulse, is studied experimentally and theoretically, as a function of the relative orientation between the laser field and the molecule. Experimentally, carbonyl sulfide, benzonitrile
Molecular chirality is an omnipresent phenomenon of fundamental significance in physics, chemistry and biology. For this reason, search for novel techniques for enantioselective control, detection and separation of chiral molecules is of particular i
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
The mixed-field orientation of an asymmetric-rotor molecule with its permanent dipole moment non-parallel to the principal axes of polarizability is investigated experimentally and theoretically. We find that for the typical case of a strong, nonreso
We explore a pure optical method for enantioselective orientation of chiral molecules by means of laser fields with twisted polarization. Several field implementations are considered, including a pair of delayed cross-polarized laser pulses, an optic