Characterizing slight structural disorder in solids by combined solid-state NMR and first principles calculations

The Journal of Physical Chemistry. a
Sylvian CadarsLyndon Emsley

Abstract

A general approach for structural interpretation of local disorder in partially ordered solids is proposed, combining high-resolution two-dimensional (2D) nuclear magnetic resonance (NMR) and first principles calculations. We show that small chemical shift variations of the order of a ppm can be interpreted in detailed structural terms with advanced density functional theory methods. Focusing on a model system of bisphosphinoamine, we demonstrate that the existence and the spatial range of small amplitude disorder can be probed using quantitative statistical analyses of 2D NMR line shapes obtained from through-space correlation experiments collected using variable mixing times. We show how low-energy vibration modes calculated from first principles can be conveniently used not as a cause of disorder but, instead, to generate a basis set of physically plausible local distortions to describe candidate static distributions of local geometries. Calculations of (31)P NMR isotropic chemical shifts are then used for the first time to simulate 2D correlation lineshapes associated with these distortions, which permit their evaluation as a potential source of disorder by comparison to experimental 2D cross-peaks between phosphorus sites....Continue Reading

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Citations

Jan 4, 2012·Journal of Pharmaceutical Sciences·Brian S LuisiBrian Moulton
May 19, 2011·Journal of Pharmaceutical Sciences·Jacalyn S ClawsonRoyston C B Copley
Jan 8, 2016·Molecular Pharmaceutics·Doris E BraunUlrich J Griesser
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Nov 29, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Vasantha GowdaPerttu Lantto
Sep 29, 2011·Physical Chemistry Chemical Physics : PCCP·Aymeric SadocFlorent Boucher
Apr 15, 2019·The Journal of Chemical Physics·Ivan Yu ChernyshovIlya G Shenderovich
Aug 5, 2009·Physical Chemistry Chemical Physics : PCCP·Anne Lesage
Feb 9, 2010·Journal of the American Chemical Society·Elodie SalagerLyndon Emsley
Apr 15, 2010·Journal of the American Chemical Society·Itzam De GortariMichele Vendruscolo
Feb 6, 2014·The Journal of Physical Chemistry Letters·Maria ConcistrèMalcolm H Levitt
Mar 13, 2014·The Journal of Physical Chemistry. B·Tomasz Pawlak, Marek J Potrzebowski
May 23, 2012·Journal of the American Chemical Society·Pierre M BeaujugeJohn R Reynolds

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