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Register a new userSpin Selection Rule-Based Sub-Millisecond Hyperpolarization of Nuclear Spins in Silicon
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In this work, we devise a fast and effective nuclear spin hyperpolarization scheme, which is in principle magnetic field and temperature independent. We use this scheme to experimentally demonstrate polarizations of up to 66% for phosphorus donor nuclear spins in bulk silicon, which are created within less than 100 us in a magnetic field of 0.35 T at a temperature of 5 K. The polarization scheme is based on a spin-dependent recombination process via weakly-coupled spin pairs, for which the recombination time constant strongly depends on the relative orientation of the two spins. We further use this scheme to measure the nuclear spin relaxation time and find a value of approx. 100 ms under illumination, in good agreement with the value calculated for nuclear spin flips induced by repeated ionization and deionization processes.
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We investigate the low-field relaxation of nuclear hyperpolarization in undoped and highly doped silicon microparticles at room temperature following removal from high field. For nominally undoped particles, two relaxation time scales are identified for ambient fields above 0.2 mT. The slower, T_1s, is roughly independent of ambient field; the faster, T_1f, decreases with increasing ambient field. A model in which nuclear spin relaxation occurs at the particle surface via a two-electron mechanism is shown to be in good agreement with the experimental data, particularly the field-independence of T_1s. For boron-doped particles, a single relaxation time scale is observed. This suggests that for doped particles, mobile carriers and bulk ionized acceptor sites, rather than paramagnetic surface states, are the dominant relaxation mechanisms. Relaxation times for the undoped particles are not affected by tumbling in a liquid solution.
Here we propose and analyse in detail protocols that can achieve rapid hyperpolarization of 13C nuclear spins in randomly oriented ensembles of nanodiamonds at room temperature. Our protocols exploit a combination of optical polarization of electron spins in nitrogen-vacancy centers and the transfer of this polarization to 13C nuclei by means of microwave control to overcome the severe challenges that are posed by the random orientation of the nanodiamonds and their nitrogen-vacancy centers. Specifically, these random orientations result in exceedingly large energy variations of the electron spin levels that render the polarization and coherent control of the nitrogen-vacancy center electron spins as well as the control of their coherent interaction with the surrounding 13C nuclear spins highly inefficient. We address these challenges by a combination of an off-resonant microwave double resonance scheme in conjunction with a realization of the integrated solid effect which, together with adiabatic rotations of external magnetic fields or rotations of nanodiamonds, leads to a protocol that achieves high levels of hyperpolarization of the entire nuclear-spin bath in a randomly oriented ensemble of nanodiamonds even at room temperature. This hyperpolarization together with the long nuclear spin polarization lifetimes in nanodiamonds and the relatively high density of 13C nuclei has the potential to result in a major signal enhancement in 13C nuclear magnetic resonance imaging and suggests functionalized and hyperpolarized nanodiamonds as a unique probe for molecular imaging both in vitro and in vivo.
Low-field (6-110 mT) magnetic resonance of bismuth (Bi) donors in silicon has been observed by monitoring the change in photoconductivity induced by spin dependent recombination. The spectra at various resonance frequencies show signal intensity distributions drastically different from that observed in conventional electron paramagnetic resonance, attributed to different recombination rates for the forty possible combinations of spin states of a pair of a Bi donor and a paramagnetic recombination center. An excellent tunability of Bi excitation energy for the future coupling with superconducting flux qubits at low fields has been demonstrated.
The elimination of defects from SiC has facilitated its move to the forefront of the optoelectronics and power-electronics industries. Nonetheless, because the electronic states of SiC defects can have sharp optical and spin transitions, they are increasingly recognized as a valuable resource for quantum-information and nanoscale-sensing applications. Here, we show that individual electron spin states in highly purified monocrystalline 4H-SiC can be isolated and coherently controlled. Bound to neutral divacancy defects, these states exhibit exceptionally long ensemble Hahn-echo spin coherence, exceeding 1 ms. Coherent control of single spins in a material amenable to advanced growth and microfabrication techniques is an exciting route to wafer-scale quantum technologies.
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.
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