The exploration of nonlinear optical crystals with ultraviolet (UV) transparent ranges and easy-to-grow large-size crystals is one of the current research interests. Herein, by combining borate and phosphate groups, a novel congruently melting alkali-mixed metal borophosphate, Li3Na7B4P6O26 (LNBPO) with UV transparency was successfully designed and synthesized using a high-temperature flux method. LNBPO crystallizes in the non-centrosymmetric (NCS) and polar orthorhombic space group Pca21 (no. 29), showcasing interesting (B2P3O13)∞ chains along the c axis. Notably, LNBPO has a moderate second harmonic generation (SHG) response (∼0.38 × KDP) and displays a wide transmission ranging from 0.22 to 3.68 μm, as measured by a [001]-oriented crystal wafer. Furthermore, a high-quality single crystal of LNBPO with sizes up to 14 × 14 × 12 mm3 was grown using the top-seeded solution growth method. The refractive indices of LNBPO were determined by applying the minimum deviation angle method. These results show that LNBPO possesses a phase-matching wavelength as short as 483 nm, indicating its potential as a new UV NLO crystal.
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