Ellipticity of High-Order Harmonics Generated by Aligned Homonuclear Diatomic Molecules Exposed to an Orthogonal Two-Color Laser Field

Abstract

We investigate emission rate and ellipticity of high-order harmonics generated exposing a homonuclear diatomic molecule, aligned in the laser-field polarization plane, to a strong orthogonally polarized two-color (OTC) laser field. The linearly polarized OTC-field components have frequencies rω and sω, where r and s are integers. Using the molecular strong-field approximation with dressed initial state and undressed final state, we calculate the harmonic emission rate and harmonic ellipticity for frequency ratios 1:2 and 1:3. The obtained quantities depend strongly on the relative phase between the laser-field components. We show that with the OTC field it is possible to generate elliptically polarized high-energy harmonics with high emission rate. To estimate the relative phase for which the emission rate is maximal we use the simple man’s model. In the harmonic spectra as a function of the molecular orientation there are two types of minima, one connected with the symmetry of the molecular orbital and the other one due to destructive interference between different contributions to the recombination matrix element, where we take into account that the electron can be ionized and recombine at the same or different atomic centers. We derive a condition for the interference minima. These minima are blurred in the OTC field except in the cases where the highest occupied molecular orbital is modeled using only s or only p orbitals in the linear combination of the atomic orbitals. This allows us to use the interference minima to assess which atomic orbitals are dominant in a particular molecular orbital. Finally, we show that the harmonic ellipticity, presented in false colors in the molecular-orientation angle vs. harmonic-order plane, can be large in particular regions of this plane. These regions are bounded by the curves determined by the condition that the harmonic ellipticity is approximately zero, which is determined by the minima of the T-matrix contributions parallel and perpendicular to the fundamental component of the OTC field.