Na2BaMQ4 (M=Ge, Sn; Q=S, Se): Infrared Nonlinear Optical Materials with Excellent Performances and that Undergo Structural Transformations

Abstract Infrared nonlinear optical (IR NLO) materials with excellent performances are particularly important in laser technology. However, to design and synthesize an efficient IR NLO material with a balance between the optical band gap and the NLO coefficient is still a huge challenge. With this in mind, four new IR NLO materials Na 2 BaSnS 4 , Na 2 BaSnSe 4 , Na 2 BaGeS 4 , and Na 2 BaGeSe 4 were successfully designed and synthesized. The compounds exhibit excellent properties with a suitable balance of band gap and NLO coefficient measured for Na 2 BaSnS 4 (3.27 eV and about 17×KDP, that is, about 17 times that of KH 2 PO 4 (KDP)) and Na 2 BaGeS 4 (3.7 eV and about 10×KDP), demonstrating that the systems satisfy the key requirements as promising IR NLO candidates. Remarkably, the new compounds also undergo a novel structural transformation from tetragonal to trigonal systems, the first time that this has been reported for quaternary metal chalcogenides.