Full-Scale Ab Initio Simulation of Magic-Angle-Spinning Dynamic Nuclear Polarization
| Autor: | Dooman Akbarian, Frédéric A. Perras, Adri C. T. van Duin, Aaron J. Rossini, Scott L. Carnahan, Marek Pruski, Muralikrishna Raju |
|---|---|
| Rok vydání: | 2020 |
| Předmět: |
Silicon
Proton Magnetic Resonance Spectroscopy Theoretical models Full scale Ab initio 02 engineering and technology Solid material Molecular Dynamics Simulation 010402 general chemistry 01 natural sciences Isotopes Magic angle spinning General Materials Science Computer Simulation Physical and Theoretical Chemistry Quantum Physics 021001 nanoscience & nanotechnology Polarization (waves) 0104 chemical sciences Computational physics Models Chemical Spin diffusion 0210 nano-technology Monte Carlo Method Hydrogen |
| Zdroj: | The journal of physical chemistry letters. 11(14) |
| ISSN: | 1948-7185 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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