Physical Chemistry

Pulse Shaped Dynamic Nuclear Polarization Under Magic Angle Spinning

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Abstract

In this paper, we report on an entirely novel way of improving the MAS-DNP efficiency by shaped μw pulse train irradiation for fast and broad-banded (FAB) saturation of the electron spin resonance. FAB-DNP achieved with Arbitrary Wave Generated shaped μw pulse trains facilitates effective and selective saturation of a defined fraction of the total electron spins, and provides superior control over the DNP efficiency under MAS. Experimental and quantum-mechanics based numerically simulated results together demonstrate that FAB-DNP significantly outperforms CW-DNP when the EPR-line of PAs is broadened by conformational distribution and exchange coupling. We demonstrate that the maximum benefit of FAB DNP is achieved when the electron spin-lattice relaxation is fast relative to the MAS frequency, i.e. at higher temperatures and/or when employing metals as PAs. Calculations predict that under short T1e conditions AWG-DNP can achieve as much as ~4-fold greater enhancement compared to CW-DNP.

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