A chemical cosubstitution strategy was implemented to design potential ultraviolet (UV) and deep-UV nonlinear optical (NLO) materials. Taking the classic β-BaB2O4 as a maternal structure, by simultaneously replacing the Ba2+ and [B3O6]3– units with monovalant (K+), divalent (alkaline earth metal), trivalent (rare-earth metal, Bi3+) ions, and the [B5O10]5– clusters through two different practical routes, 12 new mixed-metal noncentrosymmetric borates K7MIIRE2(B5O10)3 (MII = Ca, Sr, Ba, K/RE0.5; RE = Y, Lu, Gd) as well as K7MIIBi2(B5O10)3 (MII = Pb, Sr) were successfully designed and synthesized as high-quality single crystals. The selected K7CaY2(B5O10)3, K7SrY2(B5O10)3, and K7BaY2(B5O10)3 compounds were subjected to experimental and theoretical characterizations. They all exhibit suitable second-harmonic generation (SHG) responses, as large as that of commercial KH2PO4 (KDP), and also exhibit short UV cutoff edges. These results confirm the feasibility of this chemical cosubstitution strategy to design NLO...

Chemical Cosubstitution-Oriented Design of Rare-Earth Borates as Potential Ultraviolet Nonlinear Optical Materials.

A new borate LiBa3 (OH)[B9 O16 ][B(OH)4 ], which combines the uniform porosity of open-frameworks with the extraordinary NLO properties of borates, has been obtained under hydrothermal conditions by using mixed lithium and barium ions as templates. The framework displays an acs-type net with large 21-ring channels. The second harmonic generation (SHG) measurement shows that it is a type I phase-matchable material with a strong SHG signal intensity about 3.1 times that of KDP (KH2 PO4 ). UV/Vis-NIR diffuse reflectance analysis indicates that the compound has a wide transparency range with the short-wavelength absorption edge below 200 nm. These characteristics reveal that the compound is a promising deep-UV nonlinear optical material.

Deep-Ultraviolet Nonlinear Optics in a Borate Framework with 21-Ring Channels

A novel noncentrosymmetric calcium borate, Ca2[B5O9]·(OH)·H2O (1), was synthesized under solvothermal condition using mixed solvents of pyridine and H2O. Compound 1 crystallizes in the monoclinic space group Cc. Its structure contains [B5O12] units and features a three-dimensional (3D) pcu net with nine-membered ring (9-MR) channels along the b-axis, where the Ca2+ cations, OH– ions, and H2O molecules are located. Each Ca polyhedron shares three edges and one vertex with four neighbors to form a 3D dia Ca–O network. The pcu B–O net and dia Ca–O net are further interpenetrated to give the final denser net. The second harmonic generation (SHG) measurement shows that compound 1 is a type I phase-matchable material with a strong SHG response of ∼3 times that of KH2PO4. In addition, it exhibits a wide transparency range with a short UV cutoff edge below 200 nm. These results reveal that the compound is a potential deep-UV nonlinear optical material. The Vienna ab initio theoretical studies indicate the good SH...

An acentric calcium borate Ca2[B5O9]·(OH)·H2O: synthesis, structure, and nonliner optical property.

One of society’s grand challenges is to reduce energy usage in ways that are cost-effective, sustainable, and environmentally benign. Replacing incandescent and compact fluorescent light bulbs with...

Evaluating Thermal Quenching Temperature in Eu3+-Substituted Oxide Phosphors via Machine Learning.

Two non-centrosymmetric alkaline-earth metal borates, Ca2[B5O8(OH)]2[B(OH)3]·H2O (1) and Ba2[B6O9(OH)2][B3O3(OH)4]·(OH)·4H2O (2), have been synthesized under solvothermal conditions Both of them exhibit layered structures constructed from two fundamental building blocks (FBBs), respectively 1 features porous double-layers made by the acentric single A-layer and B-layer in a face-to-face arrangement Ca-O layers gather the B-O double-layers together resulting in the chiral structure of 1 Compound 2 contains two different FBBs, which is rare in borate Hexaborate B6 clusters are responsible for the expansion of inorganic B6-layers while the isolated triborate B3 clusters are arranged in supermolecular B3-layers Ba1-B6-layers and Ba2-B3-layers are alternately arranged in the same direction generating the NCS structure of 2 Both 1 and 2 are phase-matchable materials with second-harmonic generation (SHG) responses of ∼13 and ∼08 times that of KDP (KH2PO4), respectively UV-vis diffuse reflectance spectra reveal that they have short cut-off edges lower than 200 nm These characteristics make them potential deep-UV NLO materials The calculations reveal that the SHG efficiency mainly originates from the synergistic effect of the distorted MOn (M = Ca, Ba; n = 7, 10, 11) polyhedra and the asymmetric π-conjugated of BO3 units

Two deep-ultraviolet nonlinear optical alkaline-earth metal borates based on different types of oxoboron clusters

Three new mixed-metal borates, K4Ba2[B14O20(OH)10]·3H2O (1), LiSr2[B10O16(OH)3] (2), and LiBa[B9O15] (3), have been made under hydro(solvo)thermal conditions and characterized by means of IR, UV–vis–near-IR, thermogravimetric analysis, powder X-ray diffraction, and single-crystal X-ray diffraction, respectively. 1 is a 1D chain constructed from B14O21(OH)1010– cluster units, 2 is of a 2D layer with nine-membered-ring windows built up of B10O19(OH)39– cluster units, while 3 exhibits a 3D framework with 12-membered-ring channels composed of B3O7 cluster units.

Three new mixed-alkali- and alkaline-earth-metal borates: from 1D chain to 2D layer to 3D framework.

The crystal structures of the new borates (IV), (VII), and (IX) are determined by single crystal XRD.

Three New Mixed-Alkali- and Alkaline-Earth-Metal Borates: From 1D Chain to 2D Layer to 3D Framework.

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Three new mixed-alkali- and alkaline-earth-metal borates: from 1D chain to 2D layer to 3D framework.

Three New Mixed-Alkali- and Alkaline-Earth-Metal Borates: From 1D Chain to 2D Layer to 3D Framework.