Title
Full-Scale Ab Initio Simulation of Magic-Angle-Spinning Dynamic Nuclear Polarization
Publication Date
7-16-2020
Department
Ames Laboratory; Chemistry
Campus Units
Ames Laboratory, Chemistry
OSTI ID+
1638692
Report Number
IS-J 10223
DOI
10.1021/acs.jpclett.0c00955
Journal Title
The Journal of Physical Chemistry Letters
Volume Number
11
Issue Number
14
First Page
5655
Last Page
5660
Abstract
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. Here, 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.
DOE Contract Number(s)
AC02-07CH11358
Language
en
Publisher
Iowa State University Digital Repository, Ames IA (United States)