<i>Ab initio</i> multiscale simulation of high-order harmonic generation in solids

TLDR

High‑order‑harmonic generation (HHG) from infrared laser fields produces attosecond XUV pulses, a process well established in atoms and recently extended to solids, where harmonics up to order ≈ 30 have been observed in dielectrics. The study aims to develop an ab initio multiscale simulation framework for solid‑state high‑order‑harmonic generation. The authors construct this framework by integrating electronic structure calculations with macroscopic propagation and illumination modeling across the Brillouin zone. They find that mesoscopic effects—Brillouin‑zone sampling, pulse propagation in the dense medium, and inhomogeneous crystal illumination—strongly shape the harmonic spectra, explaining clean harmonic formation and influencing nonlinear optical processes in dense media.

Abstract

High-order-harmonic generation by a highly nonlinear interaction of infrared laser fields with matter allows for the generation of attosecond pulses in the XUV spectral regime. This process, well established for atoms, has been recently extended to the condensed phase. Remarkably well-pronounced harmonics up to order $\ensuremath{\sim}30$ have been observed for dielectrics. We establish a route toward an ab initio multiscale simulation of solid-state high-order-harmonic generation. We find that mesoscopic effects of the extended system, in particular the realistic sampling of the entire Brillouin zone, the pulse propagation in the dense medium, and the inhomogeneous illumination of the crystal, have a strong effect on the harmonic spectra. Our results provide an explanation for the formation of clean harmonics and have implications for a wide range of nonlinear optical processes in dense media.