Revealing the anisotropic charge-density-wave order of TiSe$_2$ through high harmonic generation

TL;DR

This paper presents a theoretical model explaining the anisotropic charge-density-wave order in TiSe₂ through high harmonic generation spectra, revealing asymmetries related to the CDW phase transition.

Contribution

A simplified phenomenological mean-field model is developed to interpret HHG spectra and reveal anisotropic CDW order in TiSe₂.

Findings

HHG spectra show strong asymmetry due to anisotropic CDW order

Model accurately describes harmonic intensity distribution as a function of polarization

Reveals potential of HHG spectroscopy to study CDW phases

Abstract

Titanium diselenide (TiSe$_{2}$) is a transition-metal dichalcogenide material that undergoes a charge-density-wave (CDW) transition at $T_{c}\approx 200\,\mathrm{K}$. In a recent experiment [I. Tyulnev {\it et al.}, Commun. Mater. 6, 152 (2025)], the high harmonic generation (HHG) spectra of this material has been studied, which exhibits asymmetric behavior with respect to the polarization angle of the incident light and provides a new perspective to the CDW phase transition. In this work, we work out a theoretical explanation for the experimentally observed behavior of HHG spectra. We propose a simplified phenomenological mean-field model for this material, based on which the HHG spectra is calculated through the time-dependent Schr{\" o}dinger equation. This model correctly describes the measured intensity distribution of the third-, fifth-, and seventh-order harmonic generation as a function of polarization direction and reveals a strong asymmetry due to the anisotropic CDW order in the low temperature phase. Our work provides a basis for applying high harmonic spectroscopy to reveal a new perspective on the nature of CDW orders.