Hybrid quantum-classical simulations of magic angle spinning dynamic nuclear polarization in very large spin systems

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Perras, Frédéric A.
Carnahan, Scott L.
Lo, Wei-Shang
Yu, Jiaqi
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Iowa State University Digital Repository, Ames IA (United States)
Huang, Wenyu
Rossini, Aaron
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.

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Solid-state nuclear magnetic resonance can be enhanced using unpaired electron spins with a method known as dynamic nuclear polarization (DNP). Fundamentally, DNP involves ensembles of thousands of spins, a scale that is difficult to match computationally. This scale prevents us from gaining a complete understanding of the spin dynamics and applying simulations to design sample formulations. We recently developed an ab initio model capable of calculating DNP enhancements in systems of up to ∼1000 nuclei; however, this scale is insufficient to accurately simulate the dependence of DNP enhancements on radical concentration or magic angle spinning (MAS) frequency. We build on this work by using ab initio simulations to train a hybrid model that makes use of a rate matrix to treat nuclear spin diffusion. We show that this model can reproduce the MAS rate and concentration dependence of DNP enhancements and build-up time constants. We then apply it to predict the DNP enhancements in core–shell metal-organic-framework nanoparticles and reveal new insights into the composition of the particles’ shells.
This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Perras, Frédéric A., Scott L. Carnahan, Wei-Shang Lo, Charles J. Ward, Jiaqi Yu, Wenyu Huang, and Aaron J. Rossini. "Hybrid quantum-classical simulations of magic angle spinning dynamic nuclear polarization in very large spin systems." The Journal of Chemical Physics 156, no. 12 (2022): 124112., and may be found at DOI: 10.1063/5.0086530. Copyright 2022 Author(s). Posted with permission. DOE Contract Number(s): AC02-07CH11358.