Orientation-dependent high harmonic generation in ZnO

TL;DR

This paper combines theoretical and experimental approaches to study how the orientation of zinc oxide crystals influences high-harmonic generation when exposed to intense mid-infrared laser pulses, revealing symmetry-dependent effects.

Contribution

It provides the first detailed comparison between theoretical predictions and experimental results on orientation-dependent HHG in ZnO, highlighting the role of crystal anisotropy.

Findings

Harmonic spectra extend beyond the band gap.

Orientation affects harmonic intensity and symmetry.

Theoretical predictions of three-fold modulation differ from experimental four-fold symmetry.

Abstract

We theoretically and experimentally investigate orientation-dependent high-harmonic generation (HHG) in zinc oxide subjected to intense femtosecond mid-infrared (MIR) laser pulses. In agreement with past measurements from literature, we observe non-perturbative harmonic spectra with harmonics extending beyond the material band gap. The spectra depend sensitively on the orientation of the crystal with respect to the laser polarization direction. To benchmark the measurements, we performed detailed theoretical calculation of the orientation-dependent harmonic yields. The theory predicts a three-fold angular modulation of the intensity of odd-order harmonics in the (0001)-plane, which can be deduced from the symmetry of the hexagonal lattice alone, in contrast a four-fold symmetry is observed in the experiment. The theory points out the essential role of the anisotropy of the multiple band structure affecting the dynamics of electron-hole pair excitation and solid-state HHG.