Mollow sidebands in high order harmonic spectra of molecules

Opt Express. 2016 Mar 7;24(5):4689-4697. doi: 10.1364/OE.24.004689.

Abstract

Novel feature of high order harmonic generation process for molecules is presented for several molecules at their equilibrium geometries. The high order harmonic spectra reveal additional sidebands for each odd harmonic, which are a consequence of the resonant coupling of two valence orbitals, a mechanism analogous to Mollow triplets known from quantum optics. Strong modification of the high order harmonic generation process is illustrated with time frequency analysis in which there appear additional minima dependent on the Rabi frequency for the corresponding transition. The orbital coupling further leads to the modification of the electron dynamics which is presented using total electron density difference maps.