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Register a new userInvestigation of room temperature multispin-assisted bulk diamond 13C hyperpolarization at low magnetic fields
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In this work we investigated the time behavior of the polarization of bulk 13C nuclei in diamond above the thermal equilibrium. This nonthermal nuclear hyperpolarization is achieved by cross relaxation between two nitrogen related paramagnetic defect species in diamond in combination with optical pumping. The decay of the hyperpolarization at four different magnetic fields is measured. Furthermore, we use the comparison with conventional nuclear resonance measurements to identify the involved distances of the nuclear spin with respect to the defects and therefore the coupling strengths. Also, a careful look at the linewidth of the signal give valuable information to piece together the puzzle of the hyperpolarization mechanism.
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Methods of optical dynamic nuclear polarization (DNP) open the door to the replenishable hyperpolarization of nuclear spins, boosting their NMR/MRI signature by orders of magnitude. Nanodiamond powder rich in negatively charged Nitrogen Vacancy (NV) defect centers has recently emerged as one such promising platform, wherein 13C nuclei can be hyperpolarized through the optically pumped defects completely at room temperature and at low magnetic fields. Given the compelling possibility of relaying this 13C polarization to nuclei in external liquids, there is an urgent need for the engineered production of highly hyperpolarizable diamond particles. In this paper, we report on a systematic study of various material dimensions affecting optical 13C hyperpolarization in diamond particles -- especially electron irradiation and annealing conditions that drive NV center formation. We discover surprisingly that diamond annealing at elevated temperatures close to 1720C have remarkable effects on the hyperpolarization levels, enhancing them by upto 36-fold over materials annealed through conventional means. We unravel the intriguing material origins of these gains, and demonstrate they arise from a simultaneous improvement in NV electron relaxation time and coherence time, as well as the reduction of paramagnetic content, and an increase in 13C relaxation lifetimes. Overall this points to significant recovery of the diamond lattice from radiation damage as a result of the high-temperature annealing. Our work suggests methods for the guided materials production of fluorescent, 13C hyperpolarized, nanodiamonds and pathways for their use as multi-modal (optical and MRI) imaging and hyperpolarization agents.
Dynamic nuclear polarization via contact with electronic spins has emerged as an attractive route to enhance the sensitivity of nuclear magnetic resonance (NMR) beyond the traditional limits imposed by magnetic field strength and temperature. Among the various alternative implementations, the use of nitrogen vacancy (NV) centers in diamond - a paramagnetic point defect whose spin can be optically polarized at room temperature - has attracted widespread attention, but applications have been hampered by the need to align the NV axis with the external magnetic field. Here we overcome this hurdle through the combined use of continuous optical illumination and a microwave sweep over a broad frequency range. As a proof of principle, we demonstrate our approach using powdered diamond where we attain bulk 13C spin polarization in excess of 0.25 percent under ambient conditions. Remarkably, our technique acts efficiently on diamond crystals of all orientations, and polarizes nuclear spins with a sign that depends exclusively on the direction of the microwave sweep. Our work paves the way towards the use of hyperpolarized diamond particles as imaging contrast agents for biosensing and, ultimately, for the hyperpolarization of nuclear spins in arbitrary liquids brought in contact with their surface.
We report hyperpolarization of the electronic spins associated with substitutional nitrogen defects in bulk diamond crystal. Hyperpolarization is achieved by optical pumping of nitrogen vacancy centers followed by rapid cross relaxation at the energy level matching condition in a 51 mT bias field. The maximum observed donor spin polarization is 0.9 % corresponding to an enhancement by 25 compared to the thermal Boltzmann polarization. A further accumulation of polarization is impeded by an anomalous optical saturation effect that we attribute to charge state conversion processes. Hyperpolarized nitrogen donors may form a useful resource for increasing the efficiency of diamond-based dynamic nuclear polarization devices.
Hyperpolarisation at room temperature is one of the most important research fields in order to improve liquid, gas or nanoparticle tracer for Magnetic Resonance Imaging (MRI) in medical applications. In this paper we utilize nuclear magnetic resonance (NMR) to investigate the hyperpolarisation effect of negatively charged nitrogen vacancy (NV) centres on carbon-13 nuclei and their spin diffusion in a diamond single crystal close to the excited state level anti crossing (ESLAC) around 50 mT. Whereas the electron spins of the NV centre can be easily polarized in its m = 0 ground state at room temperature just by irradiation with green light , the swop of the NV electron spin polarization to a carbon-13 nuclei is a complex task. We found that the coupling between the polarized NV electron spin, the electron spin of a substitutional nitrogen impurity (P1) as well as its nitrogen-14 nuclei and the carbon-13 nuclear spin has to be considered. Here we show that through an optimization of this procedure, in about two minutes a signal to noise ratio which corresponds to a 23 hour standard measurement without hyperpolarisation and an accumulation of 460 single scans can be obtained. Furthermore we were able to identify several polarisation peaks of different sign at different magnetic fields in a region of some tens of gauss. Most of the peaks can be attributed to a coupling of the NV centres to nearby P1 centres. We present a new theoretical model in a framework of cross polarisation of a four spin dynamic model in good agreement with our experimental data. The results demonstrate the opportunities and power as well as limitations of hyperpolarisation in diamond via NV centres. We expect that the current work may have a significant impact on future applications.
One of the most remarkable properties of the nitrogen-vacancy (NV) center in diamond is that optical illumination initializes its electronic spin almost completely, a feature that can be exploited to polarize other spin species in their proximity. Here we use field-cycled nuclear magnetic resonance (NMR) to investigate the mechanisms of spin polarization transfer from NVs to 13C spins in diamond at room temperature. We focus on the dynamics near 51 mT, where a fortuitous combination of energy matching conditions between electron and nuclear spin levels gives rise to alternative polarization transfer channels. By monitoring the 13C spin polarization as a function of the applied magnetic field, we show 13C spin pumping takes place via a multi-spin cross relaxation process involving the NV- spin and the electronic and nuclear spins of neighboring P1 centers. Further, we find that this mechanism is insensitive to the crystal orientation relative to the magnetic field, although the absolute level of 13C polarization - reaching up to ~3% under optimal conditions - can vary substantially depending on the interplay between optical pumping efficiency, photo-generated carriers, and laser-induced heating.
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