Direct Deep-UV Second-Harmonic Generation in Disordered Χ<sup>2</sup>-Modulated Ferroelectric Crystals.

Wu, Yabo; Cui, Chen; Han, Guopeng; Wang, Ying; Li, Fuming; Zhang, Fangfang; Yang, Zhihua; Pan, Shilie · Adv Mater · 2025

basic_science · Level V

Where this comes from

Abstract

The generation of coherent deep-ultraviolet (DUV) radiation via nonlinear frequency conversion remains a major scientific and technological challenge in modern optics. To date, only a very limited number of nonlinear optical (NLO) crystals-such as KBBF, ABF, and quartz-have been experimentally demonstrated to support measurable direct second-harmonic generation (SHG) at wavelengths of 177 nm or shorter. There is a pressing need to develop alternative materials or strategies that enable efficient frequency conversion in the DUV region. In this work, it is reported that LiKSO<sub>4</sub> (LPS), a ferroelectric sulfate crystal with z-aligned needle-like domains, forms an intrinsically disordered χ<sup>2</sup> structure that enables DUV random quasi-phase matching (RQPM) down to 163 nm across a broad spectral range. Remarkably, under nanosecond pulsed pumping at 355 nm, an SHG output at 177 nm with an energy of 3.1 µJ and a conversion efficiency of 0.11% is achieved using an x-cut LPS crystal. This study provides experimental evidence that selecting NLO crystals compatible with RQPM offers a feasible new route for DUV frequency conversion.