Exploring new materials that meet urgent needs via advanced paradigms is still a challenge. Herein, aiming at deep-ultraviolet optical functional materials with targeted properties including deep-ultraviolet transparency and high optical properties, we report an optical materials discovery paradigm—an interlinked prediction-experiment strategy. Novel fluorooxoborate crystals in the NaB₄O₆F system are predicted successfully, which realizes a balance between deep-ultraviolet transparency and large birefringence or deep-ultraviolet phase-matching wavelengths and strong nonlinear optical response. Concurrently, the experimentally oriented preparation of a new crystal NaB₄O₆F-C2/c and the known compound NaB₄O₆F-C2 is achieved, confirming the validity of the paradigm. Further results indicate that NaB₄O₆F-C2/c is a new-generation birefringent crystal with large birefringence (0.219@193 nm) and deep-ultraviolet transparency, and the phase-matching curves of NaB₄O₆F-C2 show the shortest phase-matching wavelengths for type I and type II, 166 and 200 nm. This research has enabled the customization of functional materials with high performances via the interlinked discovery paradigm.

通过先进的范例探索满足迫切需求的新材料仍然是一个挑战。在此，针对具有目标特性（包括深紫外透明度和高光学性能）的深紫外光学功能材料，我们报告了一种光学材料发现范式——一种相互关联的预测实验策略。成功预测了NaB ₄ O ₆ F体系中的新型氟代硼酸盐晶体，实现了深紫外透明度与大双折射或深紫外相位匹配波长和强非线性光学响应之间的平衡。同时，以实验为导向制备新型晶体NaB ₄ O ₆ F- C 2 / c并得到了已知化合物NaB ₄ O ₆ F- C 2 ，证实了该范式的有效性。进一步的结果表明，NaB ₄ O ₆ F- C 2/ c是新一代双折射晶体，具有大双折射（0.219@193 nm）和深紫外透明性，NaB ₄ O ₆ F- C的相位匹配曲线图 2 显示了 I 型和 II 型的最短相位匹配波长，166 和 200 nm。这项研究通过相互关联的发现范式实现了高性能功能材料的定制。