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Two new acentric polyborates, Ba3(OH)(B9O16)[B(OH)3] and Ba2.16Pb0.84(OH)(B9O16)[B(OH)3] have been synthesized hydrothermally and their structures have been determined by single-crystal X-ray diffraction. Both crystals are isostructural and crystallize in the trigonal space group P31c (no. 159). Their structures feature a three-dimensional (3D) B9O19 framework with 6-membered-ring tunnels, in which the Ba or Pb/Ba cations and [B(OH)3] groups reside. Powder second-harmonic-generation (SHG) measurements reveal that Ba3(OH)(B9O16)[B(OH)3] and Ba2.16Pb0.84(OH)(B9O16)[B(OH)3] are type-I phase-matchable, with SHG responses of 1.1× and 1.2× KH2PO4, respectively. UV-Vis-NIR diffuse reflectance analysis indicates that Ba3(OH)(B9O16)[B(OH)3] and Pb0.29Ba2.71(OH)(B9O16)[B(OH)3] have band gaps of 5.11 and 4.65 eV, respectively. In addition, first-principles calculations were employed to elucidate the origin of the NLO properties and the relationship of structure–properties.

Experimental and ab initio studies of two UV nonlinear optical materials