A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV−13C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent13C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging.
Carbon-13 dynamic nuclear polarization in diamond via a microwave-free integrated cross effect
Color-center–hosting semiconductors are emerging as promising source materials for low-field dynamic nuclear polarization (DNP) at or near room temperature, but hyperfine broadening, susceptibility to magnetic field heterogeneity, and nuclear spin relaxation induced by other paramagnetic defects set practical constraints difficult to circumvent. Here, we explore an alternate route to color-center–assisted DNP using nitrogen-vacancy (NV) centers in diamond coupled to substitutional nitrogen impurities, the so-called P1 centers. Working near the level anticrossing condition—where the P1 Zeeman splitting matches one of the NV spin transitions—we demonstrate efficient microwave-free 13 C DNP through the use of consecutive magnetic field sweeps and continuous optical excitation. The amplitude and sign of the polarization can be controlled by adjusting the low-to-high and high-to-low magnetic field sweep rates in each cycle so that one is much faster than the other. By comparing the 13 C DNP response for different crystal orientations, we show that the process is robust to magnetic field/NV misalignment, a feature that makes the present technique suitable to diamond powders and settings where the field is heterogeneous. Applications to shallow NVs could capitalize on the greater physical proximity between surface paramagnetic defects and outer nuclei to efficiently polarize target samples in contact with the more »
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Proceedings of the National Academy of Sciences
- Page Range or eLocation-ID:
- 18334 to 18340
- Sponsoring Org:
- National Science Foundation
More Like this
Disorder and many body interactions are known to impact transport and thermalization in competing ways, with the dominance of one or the other giving rise to fundamentally different dynamical phases. Here we investigate the spin diffusion dynamics of 13 C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We focus on low-abundance, strongly hyperfine-coupled nuclei, whose role in the polarization transport we expose through the integrated impact of variable radio-frequency excitation on the observable bulk 13 C magnetic resonance signal. Unexpectedly, we find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength, which we attribute to effective carbon-carbon interactions mediated by the electronic spin ensemble. In particular, observations across the full range of hyperfine couplings indicate the nuclear spin diffusion constant takes values up to two orders of magnitude greater than that expected from homo-nuclear spin couplings.
Abstract Magneto-optical (MO) effects, viz. magnetically induced changes in light intensity or polarization upon reflection from or transmission through a magnetic sample, were discovered over a century and a half ago. Initially they played a crucially relevant role in unveiling the fundamentals of electromagnetism and quantum mechanics. A more broad-based relevance and wide-spread use of MO methods, however, remained quite limited until the 1960s due to a lack of suitable, reliable and easy-to-operate light sources. The advent of Laser technology and the availability of other novel light sources led to an enormous expansion of MO measurement techniques and applications that continues to this day (see section 1). The here-assembled roadmap article is intended to provide a meaningful survey over many of the most relevant recent developments, advances, and emerging research directions in a rather condensed form, so that readers can easily access a significant overview about this very dynamic research field. While light source technology and other experimental developments were crucial in the establishment of today’s magneto-optics, progress also relies on an ever-increasing theoretical understanding of MO effects from a quantum mechanical perspective (see section 2), as well as using electromagnetic theory and modelling approaches (see section 3) to enablemore »
We demonstrate the operation of a rotation sensor based on the nitrogen-14 ( 14 N) nuclear spins intrinsic to nitrogen-vacancy (NV) color centers in diamond. The sensor uses optical polarization and readout of the nuclei and a radio-frequency double-quantum pulse protocol that monitors 14 N nuclear spin precession. This measurement protocol suppresses the sensitivity to temperature variations in the 14 N quadrupole splitting, and it does not require microwave pulses resonant with the NV electron spin transitions. The device was tested on a rotation platform and demonstrated a sensitivity of 4.7°/ s (13 mHz/ Hz ), with a bias stability of 0.4 °/s (1.1 mHz).
Sensitive and accurate diagnostic technologies with magnetic sensors are of great importance for identifying and localizing defects of rechargeable solid batteries using noninvasive detection. We demonstrate a microwave-free alternating current (AC) magnetometry method with negatively charged NV centers in diamond based on a cross-relaxation feature between nitrogen-vacancy (NV) centers and individual substitutional nitrogen (P1) centers occurring at 51.2 mT. We apply the technique to non-destructively image solid-state batteries. By detecting the eddy-current-induced magnetic field of the battery, we distinguish a defect on the external electrode and identify structural anomalies within the battery body. The achieved spatial resolution is μμμ360μm. The maximum magnetic field and phase shift generated by the battery at the modulation frequency of 5 kHz are estimated as 0.04 mT and 0.03 rad respectively.