HgCuPS4: An Exceptional Infrared Nonlinear Optical Material with Defect Diamond-like Structure

• DOI: 10.1021/acs.chemmater.0c01258
• Publication Date: 2020-04-24T13:35:23Z
• Authors: Meng-Yue Li; Zuju Ma; Bingxuan Li; Xin-Tao Wu; Hua Lin; Qi-Long Zhu
• Keywords: 01 natural sciences; 0104 chemical sciences

Infrared nonlinear optical (IR-NLO) crystals possessing excellent comprehensive performance are highly desirable, yet their preparation remains extremely challenging. Particularly, inorganic chalcogenides with diamond-like (DL) structures provide a tunable material platform for structural design and functional control. In this work, strategy involving the construction of DL using strong polarizability metal cations has been put forward; thus, quaternary Hg-containing sulfide HgCuPS4 successfully discovered by high-temperature solid-state technology. A remarkable characteristic is three-dimensional (3D) defect framework constructed vertex-sharing alignments asymmetric building motifs (ABMs). The combination unique structure Hg2+ enables such compound to achieve phase matchability in IR range high laser-induced damage threshold (4.2 × AgGaS2) second harmonic generation response (dij = 6.5 AgGaS2), best among reported so far. Moreover, detailed local dipole moment calculations theoretical results based on length-gauge formalism elucidate that very dij value originates from combined effects distorted [HgS4], [CuS4], [PS4] ABMs, is, 3D structure. This discovery can effectively help understand other promising toward future high-performing IR-NLO applications.