Laser-Dressed Molecular Point Groups in the Kramers–Henneberger Oscillating Frame-of-Reference: Selection Rules for Higher Harmonic Generation

Abstract

Point groups of molecules in a laser, within the Kramers–Henneberger (KH) oscillating frame for laser-dressed states, is given in this work. In a Fourier series of the time-dependent potential, the zeroth-order time-average yields the point group of the laser-dressed molecule. Various laser polarizations and relative molecular orientation induce a new point group or retain the original point group. The dynamical Fourier components (KH potentials) classify as irreducibles of this new laser-dressed point group. Recurrence of unique irreducibles in the Fourier expansion dictates the dynamical symmetry of the Floquet Hamiltonian. Hence, selection rules for harmonic generation spectra are Nk ± 1 in harmonic order, where N is the number of unique irreducibles and 𝑘∈𝒩.