Abstract
Noncentrosymmetric (NCS) solids have attracted interest for their potential in ferroelectric, piezoelectric, and nonlinear optical (NLO) devices, but their synthesis remains a major challenge. In this study, the additive Li2CO3 triggers formation of an NCS precursor at an early nucleation stage, and plays a crucial role in the successful polymorphism transformation. The resultant metastable β-Sc(IO3)3 is a promising mid-infrared NLO crystal, with the strongest second-harmonic generation responses (2.2 × KTiOPO4 @ 2100 nm, 16 × KH2PO4 @ 1064 nm) and the largest optical bandgap (4.52 eV) for a rare-earth iodate, as well as sufficient birefringence (Δn = 0.219 @ 546 nm) for type I phase-matching, and wide optical transparency, which are induced by optimal alignment of the iodate anions. This study reveals the key role of additives in the growth of polar NCS solids, a discovery with implications for the strategic design of new NCS polymorphism materials with exceptional NLO properties.
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