Mollow sidebands in high order harmonic spectra of molecules.

Yuqing Xia,Agnieszka Jaron-Becker

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.

Highlights

“Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses,” Phys
In order to calculate the response of a molecule, including multi-electron effects, to an intense laser field, we make use of the time-dependent density functional theory (TDDFT)
In that Figure we present the dependence of the displacement of the first and the second-order sidebands of the 9th harmonic in N+2, aligned parallel to the polarization axis, on the electric field strength

Summary

Introduction

D. Lin, “Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses,” Phys. I. Chu, “Probing the origin of elliptical high-order harmonic generation from aligned molecules in linearly polarized laser fields,” Phys. Jaron-Becker, “Multielectron contributions in elliptically polarized high-order harmonic emission from nitrogen molecule,” Opt. Lett.

Results

Conclusion