Nanoscale Solid-State Nuclear Quadrupole Resonance Spectroscopy using Depth-Optimized Nitrogen-Vacancy Ensembles in Diamond

TL;DR

This paper optimizes nitrogen-vacancy (NV) ensemble depths in diamond for enhanced nanoscale NMR and NQR spectroscopy, enabling faster and more sensitive detection of nuclear spins in 2D materials.

Contribution

It identifies the optimal NV depth for surface NMR of statistically-polarized spins and demonstrates improved NQR sensing of boron in 2D materials using NV ensembles.

Findings

Optimal NV depth for NMR sensitivity is 5.4 nm.

Ensemble NV sensors outperform single NV in measurement time.

Successful NQR spectroscopy of boron in hexagonal boron nitride.

Abstract

Nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) spectroscopy of bulk quantum materials have provided insight into phenomena such as quantum phase criticality, magnetism, and superconductivity. With the emergence of nanoscale 2-D materials with magnetic phenomena, inductively-detected NMR and NQR spectroscopy are not sensitive enough to detect the smaller number of spins in nanomaterials. The nitrogen-vacancy (NV) center in diamond has shown promise in bringing the analytic power of NMR and NQR spectroscopy to the nanoscale. However, due to depth-dependent formation efficiency of the defect centers, noise from surface spins, band bending effects, and the depth dependence of the nuclear magnetic field, there is ambiguity regarding the ideal NV depth for surface NMR of statistically-polarized spins. In this work, we prepared a range of shallow NV ensemble layer depths and determined the ideal NV depth by performing NMR spectroscopy on statistically-polarized \fluorine{} in Fomblin oil on the diamond surface. We found that the measurement time needed to achieve an SNR of 3 using XY8-N noise spectroscopy has a minimum at an NV depth of 5.4 nm. To demonstrate the sensing capabilities of NV ensembles, we perform NQR spectroscopy on the \boron{} of hexagonal boron nitride flakes. We compare our best diamond to previous work with a single NV and find that this ensemble provides a shorter measurement time with excitation diameters as small as 4 $\mu$m. This analysis provides ideal conditions for further experiments involving NMR/NQR spectroscopy of 2-D materials with magnetic properties.