Non-perturbative high-harmonic generation in the three-dimensional Dirac semimetal Cd$_3$As$_2$

TL;DR

This paper reports the experimental observation of non-perturbative high-harmonic generation up to the seventh order in a 3D Dirac semimetal driven by terahertz pulses, revealing nonlinear intraband kinetics of Dirac fermions.

Contribution

First experimental demonstration of high-harmonic generation in a 3D Dirac semimetal driven by terahertz pulses, highlighting a universal nonlinear response mechanism.

Findings

High-harmonic generation observed up to seventh order.

Non-perturbative harmonic generation linked to intraband kinetics.

Potential for controlling nonlinear responses in Dirac and Weyl materials.

Abstract

Harmonic generation is a general characteristic of driven nonlinear systems, and serves as an efficient tool for investigating the fundamental principles that govern the ultrafast nonlinear dynamics. In atomic gases, high-harmonic radiation is produced via a three-step process of ionization, acceleration, and recollision by strong-field infrared laser. This mechanism has been intensively investigated in the extreme ultraviolet and soft X-ray regions, forming the basis of attosecond research. In solid-state materials, which are characterized by crystalline symmetry and strong interactions, yielding of harmonics has just recently been reported. The observed high-harmonic generation was interpreted with fundamentally different mechanisms, such as interband tunneling combined with dynamical Bloch oscillations, intraband thermodynamics and nonlinear dynamics, and many-body electronic interactions. Here, in a distinctly different context of three-dimensional Dirac semimetal, we report on experimental observation of high-harmonic generation up to the seventh order driven by strong-field terahertz pulses. The observed non-perturbative high-harmonic generation is interpreted as a generic feature of terahertz-field driven nonlinear intraband kinetics of Dirac fermions. We anticipate that our results will trigger great interest in detection, manipulation, and coherent control of the nonlinear response in the vast family of three-dimensional Dirac and Weyl materials.