Full-Scale Ab Initio Simulation of Magic-Angle-Spinning Dynamic Nuclear Polarization

Perras, Frédéric A.; Raju, Muralikrishna; Carnahan, Scott L.; Akbarian, Dooman; van Duin, Adri C. T.; Rossini, Aaron J.; Pruski, Marek

doi:10.1021/acs.jpclett.0c00955

Full-Scale Ab Initio Simulation of Magic-Angle-Spinning Dynamic Nuclear Polarization

Journal Article · Tue May 26 00:00:00 EDT 2020 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.0c00955· OSTI ID:1638692

^[1]; ^[2]; Carnahan, Scott L. ^[2]; Akbarian, Dooman ^[3]; ^[3]; ^[2]; ^[2]

Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Pennsylvania State Univ., University Park, PA (United States)

Theoretical models aimed at describing magic-angle-spinning (MAS) dynamic nuclear polarization (DNP) NMR have great potential in facilitating the in silico design of DNP polarizing agents and formulations. These models must typically face a trade-off between the accuracy of a strict quantum mechanical description and the need for using realistically large spin systems, for instance, using phenomenological models. In this paper, we show that the use of aggressive state-space restrictions and an optimization strategy allows full-scale ab initio MAS-DNP simulations of spin systems containing thousands of nuclei. Our simulations are shown to reproduce experimental DNP enhancements quantitatively, including their MAS rate dependence, for both frozen solutions and solid materials. They also reveal the importance of a previously unrecognized structural feature found in some polarizing agents that helps minimize the sensitivity losses imposed by the spin diffusion barrier.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1638692

Report Number(s):: IS--J-10,223

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 14 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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