Dynamic Nuclear Polarization with P1 Centers in Diamond

J Phys Chem Lett. 2024 Nov 8:11504-11509. doi: 10.1021/acs.jpclett.4c02612. Online ahead of print.

Abstract

Substitutional nitrogen impurities within the diamond lattice, known as P1 centers, have unpaired electrons that can mediate microwave driven dynamic nuclear polarization (DNP). In this paper we explore DNP of the bulk 13C spins in micrometer-sized P1 diamond particles and demonstrate a 550-fold DNP enhancement of the bulk 13C spins at room temperature in a 9 T magnetic field or 250 GHz for g ≈ 2 electrons. We study the DNP mechanisms, exploring their dependence on sample spinning frequency and microwave irradiation frequency using both continuous wave and frequency swept microwave irradiation, and discuss the results alongside recent DNP studies in the literature. Even with a modest microwave irradiation power of 160 mW from our frequency swept solid-state microwave source, we achieve a significant 13C signal enhancement, ε = 270 at room temperature. The enhancements were found to increase with the magic angle spinning (MAS) frequency, ωr/2π, and the results provide mechanistic insights into how different electron populations contribute to the observed DNP efficiency. These findings are inherently interesting and of practical importance in view of the recently reported diamond rotors fabricated from P1 high-pressure, high-temperature (HPHT) diamond.