Signature of Molecular Orbital Symmetry in High-Order Harmonic Generation by Bichromatic Circularly Polarized Laser Pulses.

Molecular orbital symmetry is shown to be an important factor in determining orders and helicities (polarizations) of high-order harmonic generation (HHG) by intense femtosecond counter-rotating bichromatic circularly polarized laser pulses. Numerical solutions of time-dependent Schrödinger equations (TDSE) for the one-electron molecular ions H2+ and H32+ for different initial electronic states show that harmonic orders and helicities are dependent on orbital symmetries and of the net incident pulse electric field. The numerical results and properties of the harmonics are described by dynamical symmetry theory and time profile analysis of the high-order harmonics, thus confirming that orbital and laser pulse symmetry dependence are generic in HHG of molecules.