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

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

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)5655-5660
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume11
Issue number14
DOIs
StatePublished - Jul 16 2020

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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