Exploring infrared (IR) birefringent materials with both large birefringence (Δn) and wide band gaps (E g) is urgently demanded for high-power optoelectronic applications and has long been a tough challenge due to the intrinsic contradictory relationship between the two metrics. Herein, we developed a target-driven closed-loop framework in coupling with functional motif and crystal structure screening, deep learning assisted high-throughput optical property computation, targeted experiment and mechanism investigation, enabling efficient discovery of potential birefringent materials. Utilizing it, a batch of superior IR birefringent crystals containing planar [BS3]3- and/or stereochemically active lone pair (SCALP) groups ([SbS3]3-, [SnS3]4-, etc.) were identified: six with huge birefringence (Δn > 1.0) and three with both large birefringence (Δn > 0.5) and wide band gaps (E g > 3.5 eV). Remarkably, benefiting from a maximal synergy of [BS3]3- and [SbS3]3- motifs achieved by an optimal assembly of 1D [SbBS4]∞ chains, BaSbBS4 was highlighted and then validated experimentally as the most promising IR birefringent crystal, unlocking a record high birefringence in the wide-band-gap range (Δn = 0.95 & 2.70 eV). This work not only discovers new high-performance birefringent crystals but also offers a universal avenue for precise and efficient evaluation of optical functional materials.
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