Abstract

The molecular strong-field approximation is employed to study high-order harmonic generation by linear and planar polyatomic molecules exposed to an orthogonally polarized two-color laser field, which consists of two orthogonal linearly polarized components with commensurable frequencies. For such a driving field, we find that the harmonic emission rate and the shape of the spectrum strongly depend on the laser-field parameters including the relative phase and the ratio of the intensities of the two components. The values of the relative phase that correspond to the optimal harmonic emission rate, as well as the cutoff position, can be assessed using a classical model. The possible production of an isolated attosecond pulse is investigated. For suitable symmetry of the laser field an attosecond pulse train with only one attosecond pulse per cycle can be generated. Depending on the frequencies of the two field components, the molecular symmetry properties and the orientation of the molecule with respect to the field, the even harmonics can be absent from the spectrum, which can be used to determine the molecular orientation. The emitted harmonics are elliptically polarized and their ellipticity depends on the molecular orientation.

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