High-order harmonic generation in polyatomic molecules induced by a bicircular laser field

Abstract

High-order harmonic generation by a bicircular field, which consists of two coplanar counter-rotating circularly polarized fields of frequency $rω$ and $sω$ ($r$ and $s$ are integers), is investigated for a polyatomic molecule. This field possesses dynamical symmetry, which can be adjusted to the symmetry of the molecular Hamiltonian and used to investigate the molecular symmetry. For polyatomic molecules having the $C_{r+s}$ symmetry only the harmonics $n=q(r+s)\pm r$, $q=1,2,\ldots$, are emitted having the ellipticity $\varepsilon_n=\pm 1$. We illustrate this using the example of the planar molecules BH$_3$ and BF$_3$, which obey the $C_3$ symmetry. We show that for the BF$_3$ molecule, similarly to atoms with a $p$ ground state, there is a strong asymmetry in the emission of high harmonics with opposite helicities. This asymmetry depends on the molecular orientation.