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Crystallographic Insights into the Crystal Structure and Intrinsic Properties of Ca12Al14O33-Type Rb3LiZn2(MoO4)4 Single Crystals.

Molybdate oxide materials have attracted considerable academic interest owing to their multifunctional optoelectronic properties and applications. However, to date, studies on the intrinsic properties of multiple molybdates have rarely been implemented. Herein, a prospective triple molybdate crystal, Rb3LiZn2(MoO4)4, with high crystalline quality was successfully grown using top-seeded solution growth (TSSG) approaches. Intriguingly, it affords a cage-like structure with the I4̅3d space group, analogous to that of Ca12Al14O33 (C12A7). The Rb3LiZn2(MoO4)4 crystal exhibits excellent thermal stability up to 603 °C, accompanied by a congruent melting nature. Simultaneously, it preserves the optical merits of a large band gap of 4.10 eV and a wide transmission window of 0.29-5.4 μm, which are superior to those of most molybdate crystals. More importantly, Raman spectroscopic measurements demonstrated that the title compound possesses an intense Raman shift located at 925 cm-1 and narrow line width, facilitating a stimulated Raman laser. In addition, first-principles calculations were also implemented to elucidate the structure-property relationships of Rb3LiZn2(MoO4)4. These observations provide an empirical platform for intuitively comprehending the underlying properties of multiple molybdates and pave the way for exploiting Raman crystals.