Highly Efficient Second/Third Harmonic Generation in van der Waals Layered Material AgScP2S6 with Anisotropic Polarization and Temperature Dependence

TL;DR

This study investigates the nonlinear optical properties of AgScP2S6, revealing exceptionally high harmonic generation efficiencies, pronounced anisotropy, and temperature stability, making it promising for advanced photonic applications.

Contribution

The paper reports the first comprehensive analysis of SHG and THG in AgScP2S6, demonstrating its superior nonlinear susceptibilities and anisotropic behavior compared to other 2D materials.

Findings

High nonlinear susceptibilities: khi(2) ~ 10^(-8) m/V, khi(3) ~ 10^(-17) m^2/V^2

Pronounced anisotropic polarization-dependent harmonic generation

Temperature stability with exponential decay in harmonic signals from 300K to 25K

Abstract

Single-crystal X-ray diffraction and nonlinear optical measurements, especially second- and third-harmonic generation (SHG/THG) are comprehensively investigated for the van der Waals layered material AgScP2S6 with a non-centrosymmetric P31c (159) space group. Linear optical constants are extracted using spectroscopic ellipsometry and applied in fitting the harmonic generation behavior. Polarization-resolved SHG and THG measurements exhibit pronounced anisotropy, with emission patterns well-described by theoretical models derived from the khi(2) and khi(3) tensor elements. The material demonstrates exceptionally high nonlinear susceptibilities, with khi(2) ~ 10^(-8) m/V and khi(3) ~ 10^(-17) m^2/V^2 which is a few orders of magnitude greater than comparable 2D materials reported in the literature. Temperature-dependent SHG and THG measurements from 300 K to 25 K reveal exponential decay in harmonic signal intensities, attributed to reduced carrier mobility, with no evidence of structural phase transitions, consistent with results from single crystal diffraction and heat capacity measurements. Polarization-resolved SHG and THG measurements also reveal distinct orientation and ellipticity trends, highlighting the anisotropic nonlinear tensor contributions and contrasting polarization selection rules in the material. These results establish AgScP2S6 as a high-performance, thermally stable, and highly anisotropic nonlinear candidate material suitable for compact photonic applications such as ultrafast optical modulators, polarization-sensitive detectors, and wavelength-tunable light sources.