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Multinuclear Magnetic Resonance Crystallographic Structure Refinement and Cross-Validation Using Experimental and Computed Electric Field Gradients: Application to Na2Al2B2O7

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    Multinuclear Magnetic Resonance Crystallographic Structure Refinement and Cross-Validation Using Experimental and Computed Electric Field Gradients: Application to Na2Al2B2O7
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    Department of Chemistry and Centre for Catalysis Research and Innovation, University of Ottawa, 10 Marie Curie Private, Ottawa, Ontario, K1N 6N5, Canada
    *E-mail: [email protected]; phone 1-613-562-5800 ext 2018; fax 1-613-562-5170.
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2012, 116, 36, 19472–19482
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    https://doi.org/10.1021/jp308273h
    Published August 22, 2012
    Copyright © 2012 American Chemical Society
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    Abstract

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    An NMR crystallographic method is presented for the refinement of structures using electric field gradient (EFG) tensors measured using solid-state NMR spectroscopy and those calculated using the projector-augmented wave DFT method. As the calculated EFG data often overestimate the experimental data, the former are scaled to yield optimal agreement for a test set of compounds having highly accurate NMR data. A least-squares optimization procedure is then performed to minimize the difference between the experimental and the scaled calculated EFG tensors. This procedure yields high-quality crystal structures comparable to those obtained from pure DFT energy minimizations, as judged by their rmsd from single-crystal X-ray structures, and is based on experimental observables. Further improvement is obtained by simultaneously refining the structures against the experimental EFG tensor parameters and optimizing the lattice energy with DFT. We use this hybrid experimental–theoretical approach to refine the crystal structure of Na2Al2B2O7, a member of an important family of nonlinear optical materials, which has been the focus of study due to its tendency to form stacking faults. The resulting structures are subjected to a systematic cross-validation process using experimental 23Na, 11B, 17O, and 27Al EFG and chemical shift data, thereby demonstrating the validity of our strategy. This approach may be useful for the refinement of crystal structures of intrinsically polycrystalline materials for which typically only low quality structures are obtainable through traditional diffraction-based methods.

    Copyright © 2012 American Chemical Society

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    Comparison of the fractional coordinates for all the structures mentioned in the text, PXRD data, supplementary figures associated with the optimization of the structures of α-Al2O3 and NABO, and spectra acquired at multiple temperatures. This material is available free of charge via the Internet at http://pubs.acs.org.

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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2012, 116, 36, 19472–19482
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp308273h
    Published August 22, 2012
    Copyright © 2012 American Chemical Society
    Request reuse permissions

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