Abstract
Nonlinear-optical (NLO) metal aluminium phosphate crystal materials with deep-ultraviolet (DUV) transparent ability remain greatly unexplored. Herein, mixed alkali/alkaline-earth metal aluminium phosphate DUV NLO crystal Na2Ca17Al2(PO4)14 was successfully synthesized through the high-temperature molten technology. Na2Ca17Al2(PO4)14 features a 3D Ca-cluster-constructed framework by the stacking of Ca6O36 and (Ca/Na)3O19 clusters, which is filled by isolated Al(PO4)6 clusters and isolated PO4 tetrahedra. Na2Ca17Al2(PO4)14 exhibits a short UV absorption edge below 190 nm, phase-matching behavior with strong NLO effect of 0.9 × KDP, high thermal stability. First-principles calculations indicate that the optical properties of Na2Ca17Al2(PO4)14 derive primarily from the Ca−O groups, rather than Al–O and P–O traditional groups. The work may further promote the exploration of new DUV NLO aluminium phosphate crystal materials.
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