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

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† Key Laboratory of Functional Materials and Devices for Special Environments, Xinjiang Technical Institute of Physics & Chemistry, Chinese Academy of Sciences; Xinjiang Key Laboratory of Electronic Information Materials and Devices, 40-1 South Beijing Road, Urumqi 830011, China
‡ University of the Chinese Academy of Sciences, Beijing 100049, China
§ Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matter Physics, College of Physical Science and Technology, Yili Normal University, Yining, Xinjiang 835000, China
∥ Chemistry Department, King Fahd University of Petroleum and Minerals (KFUPM), Dhahran 31261, Kingdom of Saudi Arabia
*[email protected]
*[email protected]
*[email protected]
Cite this: J. Am. Chem. Soc. 2017, 139, 50, 18397–18405
Publication Date (Web):November 21, 2017
https://doi.org/10.1021/jacs.7b11263
Copyright © 2017 American Chemical Society
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Abstract

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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 materials and that the three selected crystals may have potential application as UV NLO materials.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.7b11263.

  • Atomic coordinates and equivalent isotropic displacement parameters, selected bond lengths for K7MIIRE2(B5O10)3 (MII = Ca, Sr, Ba, K/RE0.5; RE = Y, Lu, Gd) and K7MIIBi2(B5O10)3 (MII = Pb, Sr); experimental powder-XRD patterns and calculated band structures for K7CaY2(B5O10)3, K7SrY2(B5O10)3, K7BaY2(B5O10)3; structural evolution from Ba2Mg(BO3)2 to Ba2Mg(B3O6)2 (PDF)

  • X-ray crystallographic file in CIF format; checkcif files (ZIP)

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