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Title: Linear-scaling ab initio simulations of spin diffusion in rotating solids

Abstract

We investigated the utility of locally restricting the basis sets involved in low-order correlations in Liouville space (LCL) calculations of spin diffusion. Using well-known classical models of spin diffusion, we describe a rationale for selecting the optimal basis set for such calculations. We then show that the use of these locally restricted basis sets provides the same computational accuracy as the full LCL set while reducing the computational time by several orders of magnitude. Speeding up the calculations also enables us to use higher maximum spin orders and increase the computational accuracy. Here, unlike exact and full LCL calculations, locally restricted LCL calculations scale linearly with the system size and should thus enable the ab initio study of spin diffusion in spin systems containing several thousand spins.

Authors:
ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Ames Lab., Ames, IA (United States)
  2. Ames Lab. and Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1545356
Alternate Identifier(s):
OSTI ID: 1543056
Report Number(s):
IS-J-9961
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 3; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Perras, Frédéric A., and Pruski, Marek. Linear-scaling ab initio simulations of spin diffusion in rotating solids. United States: N. p., 2019. Web. doi:10.1063/1.5099146.
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Perras, Frédéric A., & Pruski, Marek. Linear-scaling ab initio simulations of spin diffusion in rotating solids. United States. https://doi.org/10.1063/1.5099146
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Perras, Frédéric A., and Pruski, Marek. Thu . "Linear-scaling ab initio simulations of spin diffusion in rotating solids". United States. https://doi.org/10.1063/1.5099146. https://www.osti.gov/servlets/purl/1545356.
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@article{osti_1545356,
title = {Linear-scaling ab initio simulations of spin diffusion in rotating solids},
author = {Perras, Frédéric A. and Pruski, Marek},
abstractNote = {We investigated the utility of locally restricting the basis sets involved in low-order correlations in Liouville space (LCL) calculations of spin diffusion. Using well-known classical models of spin diffusion, we describe a rationale for selecting the optimal basis set for such calculations. We then show that the use of these locally restricted basis sets provides the same computational accuracy as the full LCL set while reducing the computational time by several orders of magnitude. Speeding up the calculations also enables us to use higher maximum spin orders and increase the computational accuracy. Here, unlike exact and full LCL calculations, locally restricted LCL calculations scale linearly with the system size and should thus enable the ab initio study of spin diffusion in spin systems containing several thousand spins.},
doi = {10.1063/1.5099146},
journal = {Journal of Chemical Physics},
number = 3,
volume = 151,
place = {United States},
year = {2019},
month = {7}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5099146
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Cited by: 2 works
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Figures / Tables:

Figure 1 Figure 1: The structure of the neighbor list for a hypothetical 6-spin system (a) is shown in (b) for an Nmax value of 3. The three nearest neighbors of each spin are listed in decreasing order. This is done to avoid double counting certain dipolar couplings as we loop throughmore » the neighbor list. When a neighbor's index is lower than the central spin's index it is ignored; these are marked in red. The basis set for this spin system, with qmax set to 3, is listed in (c). Note that only the operators where each spin is found in the neighbor list of the others are included.« less
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Works referenced in this record:

Polynomially scaling spin dynamics simulation algorithm based on adaptive state-space restriction
journal, December 2007

  • Kuprov, Ilya; Wagner-Rundell, Nicola; Hore, P. J.
  • Journal of Magnetic Resonance, Vol. 189, Issue 2
  • DOI: 10.1016/j.jmr.2007.09.014

Spinach – A software library for simulation of spin dynamics in large spin systems
journal, February 2011

  • Hogben, H. J.; Krzystyniak, M.; Charnock, G. T. P.
  • Journal of Magnetic Resonance, Vol. 208, Issue 2
  • DOI: 10.1016/j.jmr.2010.11.008

Many-body kinetics of dynamic nuclear polarization by the cross effect
journal, March 2018

FT NMR of nonequilibrium states of complex spin systems. I. A Lionville space description
journal, January 1978

Multiple‐quantum dynamics in solid state NMR
journal, September 1985

  • Baum, J.; Munowitz, M.; Garroway, A. N.
  • The Journal of Chemical Physics, Vol. 83, Issue 5
  • DOI: 10.1063/1.449344

Dynamic Nuclear Polarization as Kinetically Constrained Diffusion
journal, July 2015

Fast and accurate MAS–DNP simulations of large spin ensembles
journal, January 2017

  • Mentink-Vigier, Frédéric; Vega, Shimon; De Paëpe, Gaël
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 5
  • DOI: 10.1039/c6cp07881h

NMR in rotating solids
journal, April 1979

  • Maricq, M. Matti; Waugh, J. S.
  • The Journal of Chemical Physics, Vol. 70, Issue 7
  • DOI: 10.1063/1.437915

Dynamic Nuclear Polarization NMR Spectroscopy of Microcrystalline Solids
journal, September 2012

  • Rossini, Aaron J.; Zagdoun, Alexandre; Hegner, Franziska
  • Journal of the American Chemical Society, Vol. 134, Issue 40
  • DOI: 10.1021/ja308135r

Diagonalization-free implementation of spin relaxation theory for large spin systems
journal, March 2011

Large-scale NMR simulations in liquid state: A tutorial
journal, November 2017

  • Kuprov, Ilya
  • Magnetic Resonance in Chemistry, Vol. 56, Issue 6
  • DOI: 10.1002/mrc.4660

A master-equation approach to the description of proton-driven spin diffusion from crystal geometry using simulated zero-quantum lineshapes
journal, January 2011

  • Dumez, Jean-Nicolas; Emsley, Lyndon
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 16
  • DOI: 10.1039/c1cp00004g

REPULSION, A Novel Approach to Efficient Powder Averaging in Solid-State NMR
journal, March 1997

14 N overtone NMR spectra under magic angle spinning: Experiments and numerically exact simulations
journal, February 2013

  • O’Dell, Luke A.; Brinkmann, Andreas
  • The Journal of Chemical Physics, Vol. 138, Issue 6
  • DOI: 10.1063/1.4775592

A Cog-Wheel Model for Nuclear-Spin Propagation in Solids
journal, January 1997

  • Brüschweiler, R.; Ernst, R. R.
  • Journal of Magnetic Resonance, Vol. 124, Issue 1
  • DOI: 10.1006/jmre.1996.1002

Ab initio simulation of proton spin diffusion
journal, January 2010

  • Dumez, Jean-Nicolas; Butler, Mark C.; Salager, Elodie
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 32
  • DOI: 10.1039/c0cp00050g

Optimisation of excitation schemes for 14N overtone MAS NMR using numerically exact simulations
journal, July 2017

Grid-free powder averages: On the applications of the Fokker–Planck equation to solid state NMR
journal, October 2013

  • Edwards, Luke J.; Savostyanov, D. V.; Nevzorov, A. A.
  • Journal of Magnetic Resonance, Vol. 235
  • DOI: 10.1016/j.jmr.2013.07.011

NMR crystallography of sodium diphosphates: combining dipolar, shielding, quadrupolar, diffraction, and computational information
journal, January 2013

  • Perras, Frédéric A.; Korobkov, Ilia; Bryce, David L.
  • CrystEngComm, Vol. 15, Issue 43
  • DOI: 10.1039/c3ce40875b

Large-scale ab initio simulations of MAS DNP enhancements using a Monte Carlo optimization strategy
journal, October 2018

  • Perras, Frédéric A.; Pruski, Marek
  • The Journal of Chemical Physics, Vol. 149, Issue 15
  • DOI: 10.1063/1.5042651

Quantum mechanical NMR simulation algorithm for protein-size spin systems
journal, June 2014

  • Edwards, Luke J.; Savostyanov, D. V.; Welderufael, Z. T.
  • Journal of Magnetic Resonance, Vol. 243
  • DOI: 10.1016/j.jmr.2014.04.002

Powder Crystallography by Proton Solid-State NMR Spectroscopy
journal, June 2005

  • Elena, Bénédicte; Emsley, Lyndon
  • Journal of the American Chemical Society, Vol. 127, Issue 25
  • DOI: 10.1021/ja051208t

1 H line width dependence on MAS speed in solid state NMR – Comparison of experiment and simulation
journal, June 2018

Perturbation of nuclear spin polarizations in solid state NMR of nitroxide-doped samples by magic-angle spinning without microwaves
journal, May 2014

  • Thurber, Kent R.; Tycko, Robert
  • The Journal of Chemical Physics, Vol. 140, Issue 18
  • DOI: 10.1063/1.4874341

Elucidation of cross relaxation in liquids by two-dimensional N.M.R. spectroscopy
journal, September 1980

NMR quadrupole liouvillians for arbitrary spin: Exact symbolic expressions and perturbation solutions
journal, March 2013

  • Bain, Alex D.
  • Concepts in Magnetic Resonance Part A, Vol. 42A, Issue 2
  • DOI: 10.1002/cmr.a.21259

Dynamic nuclear polarization assisted spin diffusion for the solid effect case
journal, February 2011

  • Hovav, Yonatan; Feintuch, Akiva; Vega, Shimon
  • The Journal of Chemical Physics, Vol. 134, Issue 7
  • DOI: 10.1063/1.3526486

Spin Temperature
journal, March 1958

Nanostructure of Materials Determined by Relayed Paramagnetic Relaxation Enhancement
journal, September 2015

  • Schlagnitweit, Judith; Tang, Mingxue; Baias, Maria
  • Journal of the American Chemical Society, Vol. 137, Issue 39
  • DOI: 10.1021/jacs.5b08249

Exact calculation, using angular momentum, of combined Zeeman and quadrupolar interactions in NMR
journal, November 2003

Computer-intensive simulation of solid-state NMR experiments using SIMPSON
journal, September 2014

  • Tošner, Zdeněk; Andersen, Rasmus; Stevensson, Baltzar
  • Journal of Magnetic Resonance, Vol. 246
  • DOI: 10.1016/j.jmr.2014.07.002

1H spin diffusion coefficients of highly mobile polymers
journal, November 1993

Liouvillians in NMR: The direct method revisited
journal, October 2011

Strategies for state space restriction in densely coupled spin systems with applications to spin chemistry
journal, May 2010

  • Hogben, H. J.; Hore, P. J.; Kuprov, Ilya
  • The Journal of Chemical Physics, Vol. 132, Issue 17
  • DOI: 10.1063/1.3398146

Spin diffusion in resolved solid-state NMR spectra
journal, November 1985

NMR Quantum Computation: A Critical Evaluation
journal, September 2000

SIMPSON: A General Simulation Program for Solid-State NMR Spectroscopy
journal, December 2000

  • Bak, Mads; Rasmussen, Jimmy T.; Nielsen, Niels Chr
  • Journal of Magnetic Resonance, Vol. 147, Issue 2
  • DOI: 10.1006/jmre.2000.2179

Numerical simulation of free evolution in solid-state nuclear magnetic resonance using low-order correlations in Liouville space
journal, December 2010

  • Dumez, Jean-Nicolas; Butler, Mark C.; Emsley, Lyndon
  • The Journal of Chemical Physics, Vol. 133, Issue 22
  • DOI: 10.1063/1.3505455

Molecular Structure Determination in Powders by NMR Crystallography from Proton Spin Diffusion
journal, July 2006

  • Elena, Bénédicte; Pintacuda, Guido; Mifsud, Nicolas
  • Journal of the American Chemical Society, Vol. 128, Issue 29
  • DOI: 10.1021/ja062353p

A first-principles description of proton-driven spin diffusion
journal, January 2012

  • Dumez, Jean-Nicolas; Halse, Meghan E.; Butler, Mark C.
  • Phys. Chem. Chem. Phys., Vol. 14, Issue 1
  • DOI: 10.1039/c1cp22662b

Cross relaxation and spin diffusion in the proton NMR of hydrated collagen
journal, February 1977

  • Edzes, Hommo T.; Samulski, Edward T.
  • Nature, Vol. 265, Issue 5594
  • DOI: 10.1038/265521a0

Dynamic Nuclear Polarization and Spin Diffusion in Nonconducting Solids
journal, August 2008

Exact NMR simulation of protein-size spin systems using tensor train formalism
journal, August 2014

Solid effect DNP polarization dynamics in a system of many spins
journal, March 2016

  • Wiśniewski, Daniel; Karabanov, Alexander; Lesanovsky, Igor
  • Journal of Magnetic Resonance, Vol. 264
  • DOI: 10.1016/j.jmr.2016.01.016

On the accuracy of the state space restriction approximation for spin dynamics simulations
journal, August 2011

  • Karabanov, Alexander; Kuprov, Ilya; Charnock, G. T. P.
  • The Journal of Chemical Physics, Vol. 135, Issue 8
  • DOI: 10.1063/1.3624564

Measuring Nano- to Microstructures from Relayed Dynamic Nuclear Polarization NMR
journal, July 2017

  • Pinon, Arthur C.; Schlagnitweit, Judith; Berruyer, Pierrick
  • The Journal of Physical Chemistry C, Vol. 121, Issue 29
  • DOI: 10.1021/acs.jpcc.7b04438

Dynamics of large nuclear-spin systems from low-order correlations in Liouville space
journal, August 2009

Quasi-equilibria in reduced Liouville spaces
journal, June 2012

  • Halse, Meghan E.; Dumez, Jean-Nicolas; Emsley, Lyndon
  • The Journal of Chemical Physics, Vol. 136, Issue 22
  • DOI: 10.1063/1.4726162

Macroscopic nuclear spin diffusion constants of rotating polycrystalline solids from first-principles simulation
journal, May 2015

  • Halse, Meghan E.; Zagdoun, Alexandre; Dumez, Jean-Nicolas
  • Journal of Magnetic Resonance, Vol. 254
  • DOI: 10.1016/j.jmr.2015.02.016

SPINEVOLUTION: A powerful tool for the simulation of solid and liquid state NMR experiments
journal, February 2006

Quantum mechanical simulation of solid effect dynamic nuclear polarisation using Krylov–Bogolyubov time averaging and a restricted state-space
journal, January 2012

  • Karabanov, Alexander; van der Drift, Anniek; Edwards, Luke J.
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 8
  • DOI: 10.1039/c2cp23233b

Product operator formalism for the description of NMR pulse experiments
journal, January 1984

  • Sørensen, O. W.; Eich, G. W.; Levitt, M. H.
  • Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 16
  • DOI: 10.1016/0079-6565(84)80005-9

In Silico Design of DNP Polarizing Agents: Can Current Dinitroxides Be Improved?
journal, July 2017

  • Perras, Frédéric A.; Sadow, Aaron; Pruski, Marek
  • ChemPhysChem, Vol. 18, Issue 16
  • DOI: 10.1002/cphc.201700299

QUEST—QUadrupolar Exact SofTware: A fast graphical program for the exact simulation of NMR and NQR spectra for quadrupolar nuclei
journal, July 2012

  • Perras, Frédéric A.; Widdifield, Cory M.; Bryce, David L.
  • Solid State Nuclear Magnetic Resonance, Vol. 45-46
  • DOI: 10.1016/j.ssnmr.2012.05.002

14 N overtone transition in double rotation solid-state NMR
journal, January 2015

  • Haies, Ibraheem M.; Jarvis, James A.; Brown, Lynda J.
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 37
  • DOI: 10.1039/c5cp03266k

On the interaction of nuclear spins in a crystalline lattice
journal, May 1949

Avogadro: an advanced semantic chemical editor, visualization, and analysis platform
journal, August 2012

  • Hanwell, Marcus D.; Curtis, Donald E.; Lonie, David C.
  • Journal of Cheminformatics, Vol. 4, Issue 1
  • DOI: 10.1186/1758-2946-4-17

Operator formalisms: An overview
journal, January 2006

  • Bain, Alex D.
  • Concepts in Magnetic Resonance Part A, Vol. 28A, Issue 6
  • DOI: 10.1002/cmr.a.20067

Destination state screening of active spaces in spin dynamics simulations
journal, June 2011

  • Krzystyniak, M.; Edwards, Luke J.; Kuprov, Ilya
  • Journal of Magnetic Resonance, Vol. 210, Issue 2
  • DOI: 10.1016/j.jmr.2011.03.010

Elucidation of cross relaxation in liquids by two-dimensional N.M.R. spectroscopy
journal, January 2002

Spin diffusion in resolved solid-state NMR spectra
text, January 1985

SIMPSON: A general simulation program for solid-state NMR spectroscopy
journal, December 2011

  • Bak, Mads; Rasmussen, Jimmy T.; Nielsen, Niels Chr.
  • Journal of Magnetic Resonance, Vol. 213, Issue 2
  • DOI: 10.1016/j.jmr.2011.09.008
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