Beyond Electric-Dipole Treatment of Light-Matter Interactions in Materials: Nondipole Harmonic Generation in Bulk Si

TL;DR

This paper develops a new theoretical framework to accurately simulate nondipole effects in intense light-matter interactions within bulk silicon, enabling the first first-principles nondipole harmonic generation simulations and revealing new nondipole phenomena.

Contribution

It introduces a formalism that captures nondipole effects while preserving lattice symmetry, allowing for accurate microscopic simulations of nondipole harmonic generation in materials.

Findings

First-principles nondipole harmonic generation simulation in Si.

Identification of nondipole-induced transverse currents.

Observation of nondipole high harmonic generation near damage threshold.

Abstract

A beyond electric-dipole light-matter theory is needed to describe emerging X-ray and THz applications for characterization and control of quantum materials but inaccessible as nondipole lattice-aperiodic terms impede on the use of Bloch's theorem. To circumvent this, we derive a formalism that captures dominant nondipole effects in intense electromagnetic fields while conserving lattice translational symmetry. Our approach enables the first accurate nondipole first-principles microscopic simulation of nonperturbative harmonic generation in Si. We reveal nondipole-induced transverse currents generating perturbative even-ordered harmonics and display the onset of nondipole high harmonic generation near the laser damage threshold.