“…1–4 Amongst these materials, those exhibiting acentric structures have assumed paramount significance in academic research and industrial applications due to their diverse functional attributes, including piezoelectricity, ferroelectricity, pyroelectricity, and nonlinear optical (NLO) properties. 5–10 The extensively employed NLO oxide compounds, such as borates including KBBF (KBe 2 BO 3 F 2 ), 11 β-BBO (β-BaB 2 O 4 ), 12 LBO (LiB 3 O 5 ), 13 CLBO(CsLiB 6 O 10 ) crystals, 14 and phosphates including KDP (KH 2 PO 4 ), 15 KTP (KTiOPO 4 ), 16 RTP (RbTiOPO 4 ), 17 etc ., have notably demonstrated their application in the spectral range, spanning from deep ultraviolet (UV) to near-infrared (IR). However, the relatively elevated phonon energy inherent in these materials imposes a limitation on their capacity to fabricate NLO devices that operate beyond the wavelength threshold of 4.5 μm.…”