Unearthing Superior Inorganic UV Second-Order Nonlinear Optical Materials: A Mineral-Inspired Method Integrating...

Natural minerals, with their adaptable framework structures exemplified by perovskite and lyonsite, have sparked substantial interest as potential templates for the design of advanced functional solid-state materials. Nonetheless, the quest for new materials with desired properties remains a substantial challenge, primarily due to the scarcity of effective and practical synthetic approaches. In this study, we have harnessed a synergistic approach that seamlessly integrates first-principles high-throughput screening and crystal engineering to reinvigorate the often-overlooked fresnoite mineral, Ba₂ TiOSi₂ O₇ . This innovative strategy has culminated in the successful synthesis of two superior inorganic UV nonlinear optical materials, namely Rb₂ TeOP₂ O₇ and Rb₂ SbFP₂ O₇ . Notably, Rb₂ SbFP₂ O₇ demonstrates a comprehensive enhancement in nonlinear optical performance, featuring a shortened UV absorption edge (260 nm) and a more robust second-harmonic generation response (5.1×KDP). Particularly striking is its significantly increased birefringence (0.15@546 nm), which is approximately 30 times higher than the prototype Ba₂ TiOSi₂ O₇ (0.005@546 nm). Our research has not only revitalized the potential of the fresnoite mineral for the development of new high-performance UV nonlinear optical materials but has also provided a clearly defined roadmap for the efficient exploration of novel structure-driven functional materials with targeted properties.