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

Point defects in wide-bandgap semiconductors are emerging as versatile resources for nanoscale sensing and quantum information science but our understanding of the photo-ionization 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 non-local fluorescence patterns emerging from local laser excitation, we show that in the simultaneous presence of photo-generated 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

Mechanical rotation via optical pumping of paramagnetic impurities

Hybrid quantum systems exhibiting coupled optical, spin, and mechanical degrees of freedom can serve as a platform for sensing, or as a bus to mediate interactions between qubits with disparate energy scales. These systems are also creating opportunities to test foundational ideas in quantum mechanics, including direct observations of the quantum regime in macroscopic objects. Here, we make use of angular momentum conservation to study the dynamics of a pair of paramagnetic centers featuring different spin numbers in the presence of a properly tuned external magnetic field. We examine the interplay between optical excitation, spin evolution, and mechanical motion, and theoretically show that in the presence of continuous optical illumination, interspin cross relaxation must induce rigid rotation of the host crystal. The system dynamics is robust to scattering of spin-polarized phonons, a result we build on to show this form of angular momentum transfer should be observable using state-of-the-art torsional oscillators or trapped nanoparticles.Fil: Zangara, Pablo René. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina. City College of New York; Estados UnidosFil: Wood, Alexander. University of Melbourne; AustraliaFil: Doherty, Marcus W.. Australian National University; AustraliaFil: Meriles, Carlos A.. City College of New York; Estados Unido

The Loschmidt Echo as a robust decoherence quantifier for many-body systems

We employ the Loschmidt Echo, i.e. the signal recovered after the reversal of an evolution, to identify and quantify the processes contributing to decoherence. This procedure, which has been extensively used in single particle physics, is here employed in a spin ladder. The isolated chains have 1/2 spins with XY interaction and their excitations would sustain a one-body like propagation. One of them constitutes the controlled system S whose reversible dynamics is degraded by the weak coupling with the uncontrolled second chain, i.e. the environment E. The perturbative SE coupling is swept through arbitrary combinations of XY and Ising like interactions, that contain the standard Heisenberg and dipolar ones. Different time regimes are identified for the Loschmidt Echo dynamics in this perturbative configuration. In particular, the exponential decay scales as a Fermi golden rule, where the contributions of the different SE terms are individually evaluated and analyzed. Comparisons with previous analytical and numerical evaluations of decoherence based on the attenuation of specific interferences, show that the Loschmidt Echo is an advantageous decoherence quantifier at any time, regardless of the S internal dynamics.Comment: 12 pages, 6 figure

Non-Markovian decay and dynamics of decoherence in private and public environments

We study the decay process in an open system, emphasizing on the relevance of the environment's spectral structure. Non-Markovian effects are included to quantitatively analyze the degradation rate of the coherent evolution. The way in which a two level system is coupled to different environments is specifically addressed: multiple connections to a single bath (public environment)or single connections to multiple baths (private environments). We numerically evaluate the decay rate of a local excitation by using the Survival Probability and the Loschmidt Echo. These rates are compared to analytical results obtained from the standard Fermi Golden Rule (FGR) in Wide Band Approximation, and a Self-Consistent evaluation that accounts for the bath's memory in cases where an exact analytical solution is possible. We observe that the correlations appearing in a public bath introduce further deviations from the FGR as compared with a private bath.Comment: 18 pages, 7 figures. Accepted for publication in Physical Review

Toward deep-learning-assisted spectrally-resolved imaging of magnetic noise

Recent progress in the application of color centers to nanoscale spin sensing makes the combined use of noise spectroscopy and scanning probe imaging an attractive route for the characterization of arbitrary material systems. Unfortunately, the traditional approach to characterizing the environmental magnetic field fluctuations from the measured probe signal typically requires the experimenter's input, thus complicating the implementation of automated imaging protocols based on spectrally resolved noise. Here, we probe the response of color centers in diamond in the presence of externally engineered random magnetic signals, and implement a deep neural network to methodically extract information on their associated spectral densities. Building on a long sequence of successive measurements under different types of stimuli, we show that our network manages to efficiently reconstruct the spectral density of the underlying fluctuating magnetic field with good fidelity under a broad set of conditions and with only a minimal measured data set, even in the presence of substantial experimental noise. These proof-of-principle results create opportunities for the application of machine-learning methods to color-center-based nanoscale sensing and imaging

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.Fil: Zangara, Pablo René. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina. City University of New York. The City College of New York; Estados UnidosFil: Henshaw, Jacob. City University of New York. The City College of New York; Estados UnidosFil: Pagliero, Daniela. City University of New York. The City College of New York; Estados UnidosFil: Ajoy, Ashok. Lawrence Berkeley National Laboratory; Estados Unidos. University of California at Berkeley; Estados UnidosFil: Reimer, Jeffrey A.. Lawrence Berkeley National Laboratory; Estados Unidos. University of California at Berkeley; Estados UnidosFil: Pines, Alexander. University of California at Berkeley; Estados Unidos. Lawrence Berkeley National Laboratory; Estados UnidosFil: Meriles, Carlos A.. City University of New York. The City College of New York; Estados Unidos. University of California at Berkeley; Estados Unido

13C 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 anti-crossing 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