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Issue 35, 2011
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Structural models for yttrium aluminium borate laser glasses: NMR and EPR studies of the system (Y2O3)0.2–(Al2O3)x–(B2O3)0.8−x

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Abstract

The structure of laser glasses in the system (Y2O3)0.2{(Al2O3)x)(B2O3)0.8−x} (0.15 ≤ x ≤ 0.40) has been investigated by means of 11B, 27Al, and 89Y solid state NMR as well as electron spin echo envelope modulation (ESEEM) of Yb-doped samples. The latter technique has been applied for the first time to an aluminoborate glass system. 11B magic-angle spinning (MAS)-NMR spectra reveal that, while the majority of the boron atoms are three-coordinated over the entire composition region, the fraction of three-coordinated boron atoms increases significantly with increasing x. Charge balance considerations as well as 11B NMR lineshape analyses suggest that the dominant borate species are predominantly singly charged metaborate (BO2/2O), doubly charged pyroborate (BO1/2(O)2), and (at x = 0.40) triply charged orthoborate groups. As x increases along this series, the average anionic charge per trigonal borate group increases from 1.38 to 2.91. 27Al MAS-NMR spectra show that the alumina species are present in the coordination states four, five and six, and the fraction of four-coordinated Al increases markedly with increasing x. All of the Al coordination states are in intimate contact with both the three- and the four-coordinate boron species and vice versa, as indicated by 11B/27Al rotational echo double resonance (REDOR) data. These results are consistent with the formation of a homogeneous, non-segregated glass structure. 89Y solid state NMR spectra show a significant chemical shift trend, reflecting that the second coordination sphere becomes increasingly “aluminate-like” with increasing x. This conclusion is supported by electron spin echo envelope modulation (ESEEM) data of Yb-doped glasses, which indicate that both borate and aluminate species participate in the medium range structure of the rare-earth ions, consistent with a random spatial distribution of the glass components.

Graphical abstract: Structural models for yttrium aluminium borate laser glasses: NMR and EPR studies of the system (Y2O3)0.2–(Al2O3)x–(B2O3)0.8−x

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Article information


Submitted
03 May 2011
Accepted
13 Jul 2011
First published
03 Aug 2011

Phys. Chem. Chem. Phys., 2011,13, 16071-16083
Article type
Paper

Structural models for yttrium aluminium borate laser glasses: NMR and EPR studies of the system (Y2O3)0.2–(Al2O3)x–(B2O3)0.8−x

H. Deters, J. F. de Lima, C. J. Magon, A. S. S. de Camargo and H. Eckert, Phys. Chem. Chem. Phys., 2011, 13, 16071
DOI: 10.1039/C1CP21404G

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