Spin Dynamics of a Solid-State Qubit in Proximity to a Superconductor.

A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the interplay between either system and the environment created by the color center host. Here we use a diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a superconducting film. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductor-induced redistribution of charge carriers near induced redistribution of charge carriers near the NV. We then build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the dynamics governing the spin coherence of shallow NVs, and promise opportunities for new forms of noise spectroscopy and imaging of superconductors.

Microwave-Free Dynamic Nuclear Polarization via Sudden Thermal Jumps.

Dynamic nuclear polarization (DNP) presently stands as the preferred strategy to enhance the sensitivity of nuclear magnetic resonance measurements, but its application relies on the use of high-frequency microwave to manipulate electron spins, an increasingly demanding task as the applied magnetic field grows. Here we investigate the dynamics of a system hosting a polarizing agent formed by two distinct paramagnetic centers near a level anticrossing. We theoretically show that nuclear spins polarize efficiently under a cyclic protocol that combines alternating thermal jumps and radio-frequency pulses connecting hybrid states with opposite nuclear and electronic spin alignment. Central to this process is the difference between the spin-lattice relaxation times of either electron spin species, transiently driving the electronic spin bath out of equilibrium after each thermal jump. Without the need for microwave excitation, this route to enhanced nuclear polarization may prove convenient, particularly if the polarizing agent is designed to feature electronic level anticrossings at high magnetic fields.

Optically pumped spin polarization as a probe of many-body thermalization.

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 13C 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 13C 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.

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 13C 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 13C 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 diamond crystal.

Two-Electron-Spin Ratchets as a Platform for Microwave-Free Dynamic Nuclear Polarization of Arbitrary Material Targets.

Optically pumped color centers in semiconductor powders can potentially induce high levels of nuclear spin polarization in surrounding solids or fluids at or near ambient conditions, but complications stemming from the random orientation of the particles and the presence of unpolarized paramagnetic defects hinder the flow of polarization beyond the defect's host material. Here, we theoretically study the spin dynamics of interacting nitrogen-vacancy (NV) and substitutional nitrogen (P1) centers in diamond to show that outside protons spin-polarize efficiently upon a magnetic field sweep across the NV-P1 level anticrossing. The process can be interpreted in terms of an NV-P1 spin ratchet, whose handedness, and hence the sign of the resulting nuclear polarization, depends on the relative timing of the optical excitation pulse. Further, we find that the polarization transfer mechanism is robust to NV misalignment relative to the external magnetic field, and efficient over a broad range of electron-electron and electron-nuclear spin couplings, even if proxy spins feature short coherence or spin-lattice relaxation times. Therefore, these results pave the route toward the dynamic nuclear polarization of arbitrary spin targets brought in proximity with a diamond powder under ambient conditions.

Dynamics of frequency-swept nuclear spin optical pumping in powdered diamond at low magnetic fields.

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-dependent 13C 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.

Orientation-independent room temperature optical 13C hyperpolarization in powdered diamond.

Dynamic nuclear polarization via contact with electronic spins has emerged as an attractive route to enhance the sensitivity of nuclear magnetic resonance 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. 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 with which we attain bulk 13C spin polarization in excess of 0.25% 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 toward 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.

Charge Dynamics in near-Surface, Variable-Density Ensembles of Nitrogen-Vacancy Centers in Diamond.

Although the spin properties of superficial shallow nitrogen-vacancy (NV) centers have been the subject of extensive scrutiny, considerably less attention has been devoted to studying the dynamics of NV charge conversion near the diamond surface. Using multicolor confocal microscopy, here we show that near-surface point defects arising from high-density ion implantation dramatically increase the ionization and recombination rates of shallow NVs compared to those in bulk diamond. Further, we find that these rates grow linearly, not quadratically, with laser intensity, indicative of single-photon processes enabled by NV state mixing with other defect states. Accompanying these findings, we observe NV ionization and recombination in the dark, likely the result of charge transfer to neighboring traps. Despite the altered charge dynamics, we show that one can imprint rewritable, long-lasting patterns of charged-initialized, near-surface NVs over large areas, an ability that could be exploited for electrochemical biosensing or to optically store digital data sets with subdiffraction resolution.

On-Demand Generation of Neutral and Negatively Charged Silicon-Vacancy Centers in Diamond.

Point defects in wide-band-gap semiconductors are emerging as versatile resources for nanoscale sensing and quantum information science, but our understanding of the photoionization dynamics is presently incomplete. Here, we use two-color confocal microscopy to investigate the dynamics of charge in type 1b diamond hosting nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers. By examining the nonlocal fluorescence patterns emerging from local laser excitation, we show that, in the simultaneous presence of photogenerated electrons and holes, SiV (NV) centers selectively transform into the negative (neutral) charge state. Unlike NVs, 532 nm illumination ionizes SiV^{-} via a single-photon process, thus hinting at a comparatively shallower ground state. In particular, slower ionization rates at longer wavelengths suggest the latter lies approximately ∼1.9 eV below the conduction band minimum. Building on the above observations, we demonstrate on-demand SiV and NV charge initialization over large areas via green laser illumination of variable intensity.

Loschmidt echo in many-spin systems: contrasting time scales of local and global measurements.

A local excitation in a quantum many-spin system evolves deterministically. A time-reversal procedure, involving the inversion of the signs of every energy and interaction, should produce the excitation revival. This idea, experimentally coined in nuclear magnetic resonance, embodies the concept of the Loschmidt echo (LE). While such an implementation involves a single spin autocorrelation M(1,1), i.e. a local LE, theoretical efforts have focused on the study of the recovery probability of a complete many-body state, referred to here as global or many-body LE MMB Here, we analyse the relation between these magnitudes, with regard to their characteristic time scales and their dependence on the number of spins N We show that the global LE can be understood, to some extent, as the simultaneous occurrence of N independent local LEs, i.e. MMB∼(M(1,1))(N/4) This extensive hypothesis is exact for very short times and confirmed numerically beyond such a regime. Furthermore, we discuss a general picture of the decay of M1,1 as a consequence of the interplay between the time scale that characterizes the reversible interactions (T(2)) and that of the perturbation (τ(Σ)). Our analysis suggests that the short-time decay, characterized by the time scale τ(Σ), is greatly enhanced by the complex processes that occur beyond T(2) This would ultimately lead to the experimentally observed T(3), which was found to be roughly independent of τ(Σ) but closely tied to T(2).

Time fluctuations in isolated quantum systems of interacting particles.

Numerically, we study the time fluctuations of few-body observables after relaxation in isolated dynamical quantum systems of interacting particles. Our results suggest that they decay exponentially with system size in both regimes, integrable and chaotic. The integrable systems considered are solvable with the Bethe ansatz and have a highly nondegenerate spectrum. This is in contrast with integrable Hamiltonians mappable to noninteracting ones. We show that the coefficient of the exponential decay depends on the level of delocalization of the initial state with respect to the energy shell.