Macroscopic Nuclear Spin Diffusion Constants of Rotating Polycrystalline Solids from First-Principles Simulation

Meghan E. Halse; Alexandre Zagdoun; Jean-Nicolas Dumez; Lyndon Emsley

doi:10.1016/j.jmr.2015.02.016

Macroscopic Nuclear Spin Diffusion Constants of Rotating Polycrystalline Solids from First-Principles Simulation

Meghan E. Halse, Alexandre Zagdoun, Jean-Nicolas Dumez, Lyndon Emsley

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

A method for quantitatively calculating nuclear spin diffusion constants directly from crystal structures is introduced. This approach uses the first-principles low-order correlations in Liouville space (LCL) method to simulate spin diffusion in a box, starting from atomic geometry and including both MAS and powder averaging. The LCL simulations are fit to the 3D diffusion equation to extract quantitative nuclear spin diffusion constants. We demonstrate this method for the case of 1H spin diffusion in ice and l-histidine, obtaining diffusion constants that are consistent with literature values for 1H spin diffusion in polymers and that follow the expected trends with respect to magic-angle spinning rate and the density of nuclear spins. In addition, we show that this method can be used to model 13C spin diffusion in diamond and therefore has the potential to provide insight into applications such as the transport of polarization in non-protonated systems.

Original language	English
Pages (from-to)	48-55
Number of pages	8
Journal	Journal of Magnetic Resonance
Volume	254
Early online date	7 Mar 2015
DOIs	https://doi.org/10.1016/j.jmr.2015.02.016
Publication status	Published - May 2015

Keywords

Solid-state NMR
Low-order correlations in Liouville space (LCL)
Polarisation transport
Numerical simulation

Access to Document

10.1016/j.jmr.2015.02.016

Cite this

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title = "Macroscopic Nuclear Spin Diffusion Constants of Rotating Polycrystalline Solids from First-Principles Simulation",

abstract = "A method for quantitatively calculating nuclear spin diffusion constants directly from crystal structures is introduced. This approach uses the first-principles low-order correlations in Liouville space (LCL) method to simulate spin diffusion in a box, starting from atomic geometry and including both MAS and powder averaging. The LCL simulations are fit to the 3D diffusion equation to extract quantitative nuclear spin diffusion constants. We demonstrate this method for the case of 1H spin diffusion in ice and l-histidine, obtaining diffusion constants that are consistent with literature values for 1H spin diffusion in polymers and that follow the expected trends with respect to magic-angle spinning rate and the density of nuclear spins. In addition, we show that this method can be used to model 13C spin diffusion in diamond and therefore has the potential to provide insight into applications such as the transport of polarization in non-protonated systems.",

keywords = "Solid-state NMR, Low-order correlations in Liouville space (LCL), Polarisation transport, Numerical simulation",

author = "Halse, {Meghan E.} and Alexandre Zagdoun and Jean-Nicolas Dumez and Lyndon Emsley",

year = "2015",

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doi = "10.1016/j.jmr.2015.02.016",

language = "English",

volume = "254",

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publisher = "Academic Press",

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TY - JOUR

T1 - Macroscopic Nuclear Spin Diffusion Constants of Rotating Polycrystalline Solids from First-Principles Simulation

AU - Halse, Meghan E.

AU - Zagdoun, Alexandre

AU - Dumez, Jean-Nicolas

AU - Emsley, Lyndon

PY - 2015/5

Y1 - 2015/5

N2 - A method for quantitatively calculating nuclear spin diffusion constants directly from crystal structures is introduced. This approach uses the first-principles low-order correlations in Liouville space (LCL) method to simulate spin diffusion in a box, starting from atomic geometry and including both MAS and powder averaging. The LCL simulations are fit to the 3D diffusion equation to extract quantitative nuclear spin diffusion constants. We demonstrate this method for the case of 1H spin diffusion in ice and l-histidine, obtaining diffusion constants that are consistent with literature values for 1H spin diffusion in polymers and that follow the expected trends with respect to magic-angle spinning rate and the density of nuclear spins. In addition, we show that this method can be used to model 13C spin diffusion in diamond and therefore has the potential to provide insight into applications such as the transport of polarization in non-protonated systems.

AB - A method for quantitatively calculating nuclear spin diffusion constants directly from crystal structures is introduced. This approach uses the first-principles low-order correlations in Liouville space (LCL) method to simulate spin diffusion in a box, starting from atomic geometry and including both MAS and powder averaging. The LCL simulations are fit to the 3D diffusion equation to extract quantitative nuclear spin diffusion constants. We demonstrate this method for the case of 1H spin diffusion in ice and l-histidine, obtaining diffusion constants that are consistent with literature values for 1H spin diffusion in polymers and that follow the expected trends with respect to magic-angle spinning rate and the density of nuclear spins. In addition, we show that this method can be used to model 13C spin diffusion in diamond and therefore has the potential to provide insight into applications such as the transport of polarization in non-protonated systems.

KW - Solid-state NMR

KW - Low-order correlations in Liouville space (LCL)

KW - Polarisation transport

KW - Numerical simulation

U2 - 10.1016/j.jmr.2015.02.016

DO - 10.1016/j.jmr.2015.02.016

M3 - Article

SN - 1090-7807

VL - 254

SP - 48

EP - 55

JO - Journal of Magnetic Resonance

JF - Journal of Magnetic Resonance

ER -