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Third harmonic generation in the transition metal trichalcogenides

Timothy Y. Chung, Vergil M. Schreiber, Randy M. Sterbentz, David P. Shelton, and Joshua O. Island*

Eduardo Flores

Jose Ramon Ares and Isabel J. Ferrer†

  • Departamento de Física Aplicada, Centro de Investigación y Estudios Avanzados, 97310 Mérida, México

  • *Contact author: joshua.island@unlv.edu
  • †Also at Instituto Nicolás Cabrera (INC), Universidad Autónoma de Madrid, UAM, 28049 Madrid, Spain.
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Phys. Rev. Materials 10, 104009 – Published 22 October, 2026

DOI: https://doi.org/10.1103/w38j-dmbg

Abstract

The transition metal trichalcogenides (TMTs) are an interesting class of layered 2D materials that have strong anisotropic electrical and optical properties. We report on the polarization-dependent nonlinear optical response of exfoliated crystals at the third harmonic using nonresonant excitation with a 1560 nm femtosecond laser. All members of the TMT crystal family explored (ZrS3, HfS3, TiS3, and NbS3) display large anisotropy in their polarized third harmonic generation signal, with anisotropy ratios as large as χ11/χ22≈6.5. From the expected nonlinear dependence of these monoclinic and triclinic crystals, we extract the relative nonlinear susceptibility coefficients. We find that the anisotropy ratio is largest for ZrS3 and decreases across the family, a trend we associate with the proximity of the third harmonic energy to the strongly b-polarized absorption edge of each material. NbS3, the only triclinic crystal, displays a pronounced anisotropy in thick flakes that is strongly reduced in the thinnest flakes, which we attribute to a partial relaxation of the Peierls-type Nb–Nb dimerization that underlies the triclinic distortion. The large anisotropic nonlinear response in this crystal family sets it apart from other 2D materials and makes them particularly attractive for further investigation.

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Phys. Rev. Materials 10, 104009– Published 22 October, 2026
  • Received 2 July 2026
  • Accepted 1 October 2026
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