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The charge state of a quantum point defect in a solid state host strongly determines its optical and spin characteristics. Consequently, techniques for controlling the charge state are required to realize technologies such as quantum networking and sensing. In this work we demonstrate the use of deep-ultraviolet (DUV) radiation to dynamically neutralize nitrogen- (NV) and silicon-vacancy (SiV) centers. We first examine the conversion between the neutral and negatively charged NV states by correlating the variation of their respective spectra, indicating that more than 99% of the population of NV centers can be initialized into the neutral charge state. We then examine the time dynamics of bleaching and recharging of negatively charged SiV$^-$ centers and observe an 80% reduction in SiV$^-$ photoluminescence within a single 100-$\mu$s DUV pulse. Finally we demonstrate that the bleaching of SiV$^-$ induced by the DUV is accompanied by a dramatic increase in the neutral SiV$^0$ population; SiV$^0$ remains robust to extended periods of near-infrared excitation despite being a non-equilibrium state. DUV excitation thus presents a reliable method of generating SiV$^0$, a desirable charge state for quantum network applications that is challenging to obtain by equilibrium Fermi engineering alone. Our results on two separate color centers at technologically relevant temperatures indicate a potential for above-band-gap excitation as a universal means of generating the neutral charge states of quantum point defects on demand.

DNA flexibility is a key determinant of biological function, from nucleosome positioning to transcriptional regulation, motivating a direct measurement of the bend-torque response of individual DNA molecules. In this work, DNA bending is detected using a nano-mechanical torque balance formed by tethering a ferromagnetic nanoparticle probe by an individual DNA molecule to a diamond magnetic field imager. The torque exerted by the DNA in response to bending caused by an applied magnetic torque is measured using wide-field imaging of quantum defects near the surface of the diamond. Qualitative measurements of differences in DNA bio-mechanical binding configuration are demonstrated, and as a proof-of-principle, a quantitative measurement of the bend response is made for individual DNA molecules. This quantum-enabled measurement approach could be applied to characterize the bend response of biophysically relevant short DNA molecules as well as the sequence dependence of DNA bending energy.

The need of near-surface color centers in diamond for quantum technologies motivates the controlled doping of specific extrinsic impurities into the crystal lattice. Recent experiments have shown that this can be achieved by momentum transfer from a surface precursor via ion implantation, an approach known as ``recoil implantation.'' Here, we extend this technique to incorporate dielectric precursors for creating nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers in diamond. Specifically, we demonstrate that gallium focused-ion-beam exposure to a thin layer of silicon nitride or silicon dioxide on the diamond surface results in the introduction of both extrinsic impurities and carbon vacancies. These defects subsequently give rise to near-surface NV and SiV centers with desirable optical properties after annealing.

The shallow donor in zinc oxide (ZnO) is a promising semiconductor spin qubit with optical access. Single indium donors are isolated in a commercial ZnO substrate using plasma focused ion beam (PFIB) milling. Quantum emitters are identified optically by spatial and frequency filtering. The indium donor assignment is based on the optical bound exciton transition energy and magnetic dependence. The single donor emission is intensity and frequency stable with a transition linewidth less than twice the lifetime limit. The isolation of optically stable single donors post-FIB fabrication is promising for optical device integration required for scalable quantum technologies based on single donors in direct band gap semiconductors., Comment: E. R. Hansen and V. Niaouris contributed equally to this work. 15 pages, 13 figures

Quantum technologies based on quantum point defects in crystals require control over the defect charge state. Here we tune the charge state of shallow nitrogen-vacancy and silicon-vacancy centers by locally oxidizing a hydrogenated surface with moderate optical excitation and simultaneous spectral monitoring. The loss of conductivity and change in work function due to oxidation are measured in atmosphere using conductive atomic force microscopy (C-AFM) and Kelvin probe force microscopy (KPFM). We correlate these scanning probe measurements with optical spectroscopy of the nitrogen-vacancy and silicon-vacancy centers created via implantation and annealing 15-25 nm beneath the diamond surface. The observed charge state of the defects as a function of optical exposure demonstrates that laser oxidation provides a way to precisely tune the Fermi level over a range of at least 2.00 eV. We also observe a significantly larger oxidation rate for implanted surfaces compared to unimplanted surfaces under ambient conditions. Combined with knowledge of the electron affinity of a surface, these results suggest KPFM is a powerful, high-spatial resolution technique to advance surface Fermi level engineering for charge stabilization of quantum defects.

Neutral shallow donors in zinc oxide (ZnO) are spin qubits with optical access via the donor-bound exciton. This spin-photon interface enables applications in quantum networking, memories and transduction. Essential optical parameters which impact the spin-photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth and optical depth. We study the donor-bound exciton optical linewidth properties of Al, Ga, and In donors in single-crystal ZnO. The ensemble photoluminescence linewidth ranges from 4-11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption through samples with an estimated optical depth up to several hundred. The primary thermal relaxation mechanism is identified and found to have a negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, contributing 2 GHz. Two-laser spectral hole burning measurements, indicate the dominant mechanism, however, is homogeneous. Despite this broadening, the high homogeneity, large optical depth and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies., Comment: V. Niaouris and S. H. D'Ambrosia contributed equally to this work, 24 pages, 12 figures

The compact size, scalability, and strongly confined fields in integrated photonic devices enable new functionalities in photonic networking and information processing, both classical and quantum. Gallium phosphide (GaP) is a promising material for active integrated photonics due to its high refractive index, wide band gap, strong nonlinear properties, and large acousto-optic figure of merit. In this work we demonstrate that silicon-lattice-matched boron-doped GaP (BGaP), grown at the 12-inch wafer scale, provides similar functionalities as GaP. BGaP optical resonators exhibit intrinsic quality factors exceeding 25,000 and 200,000 at visible and telecom wavelengths respectively. We further demonstrate the electromechanical generation of low-loss acoustic waves and an integrated acousto-optic (AO) modulator. High-resolution spatial and compositional mapping, combined with ab initio calculations indicate two candidates for the excess optical loss in the visible band: the silicon-GaP interface and boron dimers. These results demonstrate the promise of the BGaP material platform for the development of scalable AO technologies at telecom and provide potential pathways toward higher performance at shorter wavelengths.

Shallow neutral donors (D$^{0}$) in ZnO have emerged as a promising candidate for solid-state spin qubits. Here, we report on the formation of D$^{0}$ in ZnO via implantation of In and subsequent annealing. The implanted In donors exhibit optical and spin properties on par with $\textit{in situ}$ doped donors. The inhomogeneous linewidth of the donor-bound exciton transition is less than 10 GHz, comparable to the optical linewidth of $\textit{in situ}$ In. Longitudinal spin relaxation times ($T_1$) exceed reported values for $\textit{in situ}$ Ga donors, indicating that residual In implantation damage does not degrade $T_1$. Two laser Raman spectroscopy on the donor spin reveals the hyperfine interaction of the donor electron with the spin-9/2 In nuclei. This work is an important step toward the deterministic formation of In donor qubits in ZnO with optical access to a long-lived nuclear spin memory.

Optically addressable solid-state defects are emerging as one of the most promising qubit platforms for quantum networks. Maximizing photon-defect interaction by nanophotonic cavity coupling is key to network efficiency. We demonstrate fabrication of gallium phosphide 1-D photonic crystal waveguide cavities on a silicon oxide carrier and subsequent integration with implanted silicon-vacancy (SiV) centers in diamond using a stamp-transfer technique. The stamping process avoids diamond etching and allows fine-tuning of the cavities prior to integration. After transfer to diamond, we measure cavity quality factors ($Q$) of up to 8900 and perform resonant excitation of single SiV centers coupled to these cavities. For a cavity with $Q$ of 4100, we observe a three-fold lifetime reduction on-resonance, corresponding to a maximum potential cooperativity of $C = 2$. These results indicate promise for high photon-defect interaction in a platform which avoids fabrication of the quantum defect host crystal.

We demonstrate quasi-phase matched, triply-resonant sum frequency conversion in 10.6-um-diameter integrated gallium phosphide ring resonators. A small-signal, waveguide-to-waveguide power conversion efficiency of 8%/mW is measured for conversion from telecom (1536 nm) and near infrared (1117 nm) to visible (647 nm) wavelengths with an absolute power conversion efficiency of 6.3% measured at saturation pump power. For the complementary difference frequency generation process, a single photon conversion efficiency of 7.2%/mW from visible to telecom is projected for resonators with optimized coupling. Efficient conversion from visible to telecom will facilitate long-distance transmission of spin-entangled photons from solid-state emitters such as the diamond NV center, allowing long-distance entanglement for quantum networks., Comment: 15 pages, 5 figures

We present an experimental and theoretical study of the longitudinal electron spin relaxation ($T_1$) of shallow donors in the direct band-gap semiconductor ZnO. $T_1$ is measured via resonant excitation of the Ga donor-bound exciton. $T_1$ exhibits an inverse-power dependence on magnetic field $T_1\propto B^{-n}$, with $4\leq n\leq 5$, over a field range of 1.75 T to 7 T. We derive an analytic expression for the donor spin-relaxation rate due to spin-orbit (admixture mechanism) and electron-phonon (piezoelectric) coupling for the wurtzite crystal symmetry. Excellent quantitative agreement is found between experiment and theory suggesting the admixture spin-orbit mechanism is the dominant contribution to $T_1$ in the measured magnetic field range. Temperature and excitation-energy dependent measurements indicate a donor density dependent interaction may contribute to small deviations between experiment and theory. The longest $T_1$ measured is 480 ms at 1.75 T with increasing $T_1$ at smaller fields theoretically expected. This work highlights the extremely long longitudinal spin-relaxation time for ZnO donors due to their small spin-orbit coupling., Comment: 9 pages, 11 figures

Shallow donors in ZnO are promising candidates for photon-mediated quantum technologies. Utilizing the indium donor, we show that favorable donor-bound exciton optical and electron spin properties are retained in isolated ZnO nanowires. The inhomogeneous optical linewidth of single nanowires (60 GHz) is within a factor of 2 of bulk single-crystalline ZnO. Spin initialization via optical pumping is demonstrated and coherent population trapping is observed. The two-photon absorption width approaches the theoretical limit expected due to the hyperfine interaction between the indium nuclear spin and the donor-bound electron.

We demonstrate post-fabrication target-wavelength trimming with a gallium phosphide on silicon nitride integrated photonic platform using controlled electron-beam exposure of hydrogen silsesquioxane cladding. A linear relationship between the electron-beam exposure dose and resonant wavelength red-shift enables deterministic, individual trimming of multiple devices on the same chip to within 30 pm of a single target wavelength. Second harmonic generation from telecom to near infrared at a target wavelength is shown in multiple devices with quality factors on the order of $10^4$. Post-fabrication tuning is an essential tool for targeted wavelength applications including quantum frequency conversion

Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by $^{15}$N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths ($<$ 60 MHz) are observed for the majority of the normal-implant (7$^\circ$, $\approx$ 100 nm deep) $^{15}$NV centers. Long-term stability of the NV$^-$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85$^\circ$, $\approx$ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering., Comment: 8 pages, 6 figures, 1 table

Hole spins in semiconductors are a potential qubit alternative to electron spins. In nuclear-spin-rich host crystals like GaAs, the hyperfine interaction of hole spins with nuclei is considerably weaker than that for electrons, leading to potentially longer coherence times. Here we demonstrate optical pumping and coherent population trapping for acceptor-bound holes in a strained GaAs epitaxial layer. We find $\mu$s-scale longitudinal spin relaxation time T$_1$ and an inhomogeneous dephasing time T$_2^*$ of $\sim$7~ns. We attribute the spin relaxation mechanism to a combination effect of a hole-phonon interaction through the deformation potentials and a heavy-hole light-hole mixing in an in-plane magnetic field. We attribute the short T$_2^*$ to g-factor broadening due to strain inhomogeneity. T$_1$ and T$_2^*$ are quantitatively calculated based on these mechanisms and compared with the experimental results. While the hyperfine-mediated decoherence is mitigated, our results highlight the important contribution of strain to relaxation and dephasing of acceptor-bound hole spins.

We present an imaging modality that enables detection of magnetic moments and their resulting stray magnetic fields. We use wide-field magnetic imaging that employs a diamond-based magnetometer and has combined magneto-optic detection (e.g. magneto-optic Kerr effect) capabilities. We employ such an instrument to image magnetic (stripe) domains in multilayered ferromagnetic structures., Comment: 7 pages

State-of-the-art magnetic field measurements performed in shielded environments with carefully controlled conditions rarely reflect the realities of those applications envisioned in the introductions of peer-reviewed publications. Nevertheless, significant advances in magnetometer sensitivity have been accompanied by serious attempts to bring these magnetometers into the challenging working environments in which they are often required. This review discusses the ways in which various (predominantly optically-pumped) magnetometer technologies have been adapted for use in a wide range of noisy and physically demanding environments.

Solid-state defect qubit systems with spin-photon interfaces show great promise for quantum information and metrology applications. Photon collection efficiency, however, presents a major challenge for defect qubits in high refractive index host materials. Inverse-design optimization of photonic devices enables unprecedented flexibility in tailoring critical parameters of a spin-photon interface including spectral response, photon polarization and collection mode. Further, the design process can incorporate additional constraints, such as fabrication tolerance and material processing limitations. Here we design and demonstrate a compact hybrid gallium phosphide on diamond inverse-design planar dielectric structure coupled to single near-surface nitrogen-vacancy centers formed by implantation and annealing. We observe device operation near the theoretical limit and measure up to a 14-fold broadband enhancement in photon extraction efficiency. We expect that such inverse-designed devices will enable realization of scalable arrays of single-photon emitters, rapid characterization of new quantum emitters, sensing and efficient heralded entanglement schemes.

We propose an optical scheme to generate an entangled state between a trapped ion and a solid state donor qubit through which-path erasure of identical photons emitted from the two systems. The proposed scheme leverages the similar transition frequencies between In donor bound excitons in ZnO and the $^2P_{1/2}$ to $^2S_{1/2}$ transition in Yb$^+$. The lifetime of the relevant ionic state is longer than that of the ZnO system by a factor of 6, leading to a mismatch in the temporal profiles of emitted photons. A detuned cavity-assisted Raman scheme weakly excites the donor with a shaped laser pulse to generate photons with 0.99 temporal overlap to the Yb$^+$ emission and partially shift the emission of the defect toward the Yb$^+$ transition. The remaining photon shift is accomplished via the dc Stark effect. We show that an entanglement rate of 21 kHz and entanglement fidelity of 94 % can be attained using a weak excitation scheme with reasonable parameters.

Wide-field magnetometry can be realized by imaging the optically-detected magnetic resonance of diamond nitrogen vacancy (NV) center ensembles. However, NV ensemble inhomogeneities significantly limit the magnetic-field sensitivity of these measurements. We demonstrate a double-double quantum (DDQ) driving technique to facilitate wide-field magnetic imaging of dynamic magnetic fields at a micron scale. DDQ imaging employs four-tone radio frequency pulses to suppress inhomogeneity-induced variations of the NV resonant response. As a proof-of-principle, we use the DDQ technique to image the dc magnetic field produced by individual magnetic-nanoparticles tethered by single DNA molecules to a diamond sensor surface. This demonstrates the efficacy of the diamond NV ensemble system in high-frame-rate magnetic microscopy, as well as single-molecule biophysics applications.

Magnetic proximity effects are crucial ingredients for engineering spintronic, superconducting, and topological phenomena in heterostructures. Such effects are highly sensitive to the interfacial electronic properties, such as electron wave function overlap and band alignment. The recent emergence of van der Waals (vdW) magnets enables the possibility of tuning proximity effects via designing heterostructures with atomically clean interfaces. In particular, atomically thin CrI3 exhibits layered antiferromagnetism, where adjacent ferromagnetic monolayers are antiferromagnetically coupled. Exploiting this magnetic structure, we uncovered a layer-resolved magnetic proximity effect in heterostructures formed by monolayer WSe2 and bi/trilayer CrI3. By controlling the individual layer magnetization in CrI3 with a magnetic field, we found that the spin-dependent charge transfer between WSe2 and CrI3 is dominated by the interfacial CrI3 layer, while the proximity exchange field is highly sensitive to the layered magnetic structure as a whole. These properties enabled us to use monolayer WSe2 as a spatially sensitive magnetic sensor to map out layered antiferromagnetic domain structures at zero magnetic field as well as antiferromagnetic/ferromagnetic domains near the spin-flip transition in bilayer CrI3. Our work reveals a new way to control proximity effects and probe interfacial magnetic order via vdW engineering., Comment: to appear in Nature Nanotechnology

Quantum simulators are a promising technology on the spectrum of quantum devices from specialized quantum experiments to universal quantum computers. These quantum devices utilize entanglement and many-particle behaviors to explore and solve hard scientific, engineering, and computational problems. Rapid development over the last two decades has produced more than 300 quantum simulators in operation worldwide using a wide variety of experimental platforms. Recent advances in several physical architectures promise a golden age of quantum simulators ranging from highly optimized special purpose simulators to flexible programmable devices. These developments have enabled a convergence of ideas drawn from fundamental physics, computer science, and device engineering. They have strong potential to address problems of societal importance, ranging from understanding vital chemical processes, to enabling the design of new materials with enhanced performance, to solving complex computational problems. It is the position of the community, as represented by participants of the NSF workshop on "Programmable Quantum Simulators," that investment in a national quantum simulator program is a high priority in order to accelerate the progress in this field and to result in the first practical applications of quantum machines. Such a program should address two areas of emphasis: (1) support for creating quantum simulator prototypes usable by the broader scientific community, complementary to the present universal quantum computer effort in industry; and (2) support for fundamental research carried out by a blend of multi-investigator, multi-disciplinary collaborations with resources for quantum simulator software, hardware, and education., Comment: 41 pages -- references and acknowledgments added in v2

Two-dimensional stacking fault defects embedded in a bulk crystal can provide a homogeneous trapping potential for carriers and excitons. Here we utilize state-of-the-art structural imaging coupled with density functional and effective-mass theory to build a microscopic model of the stacking-fault exciton. The diamagnetic shift and exciton dipole moment at different magnetic fields are calculated and compared with the experimental photoluminescence of excitons bound to a single stacking fault in GaAs. The model is used to further provide insight into the properties of excitons bound to the double-well potential formed by stacking fault pairs. This microscopic exciton model can be used as an input into models which include exciton-exciton interactions to determine the excitonic phases accessible in this system., Comment: 12 pages, 10 figures

Knowledge of the nitrogen-vacancy center formation kinetics in diamond is critical to engineering sensors and quantum information devices based on this defect. Here we utilize the longitudinal tracking of single NV centers to elucidate NV defect kinetics during high-temperature annealing from 800-1100 $^\circ$C in high-purity chemical-vapor-deposition diamond. We observe three phenomena which can coexist: NV formation, NV quenching, and NV orientation changes. Of relevance to NV-based applications, a 6 to 24-fold enhancement in the NV density, in the absence of sample irradiation, is observed by annealing at 980 $^\circ$C, and NV orientation changes are observed at 1050 $^\circ$C. With respect to the fundamental understanding of defect kinetics in ultra-pure diamond, our results indicate a significant vacancy source can be activated for NV creation between 950-980 $^\circ$C and suggests that native hydrogen from NVH$_y$ complexes plays a dominant role in NV quenching, in agreement with recent {\it ab initio} calculations. Finally, the direct observation of orientation changes allows us to estimate an NV diffusion barrier of 5.1~eV.

Second harmonic conversion from 1550~nm to 775~nm with an efficiency of 400% W$^{-1}$ is demonstrated in a gallium phosphide (GaP) on oxide integrated photonic platform. The platform consists of doubly-resonant, phase-matched ring resonators with quality factors $Q \sim 10^4$, low mode volumes $V \sim 30 (\lambda/n)^3$, and high nonlinear mode overlaps. Measurements and simulations indicate that conversion efficiencies can be increased by a factor of 20 by improving the waveguide-cavity coupling to achieve critical coupling in current devices., Comment: 13 pages, 6 figures

Monolayer valley semiconductors, such as tungsten diselenide (WSe$_2$), possess valley pseudospin degrees of freedom that are optically addressable but degenerate in energy. Lifting the energy degeneracy by breaking time-reversal symmetry is vital for valley manipulation. This has been realized by directly applying magnetic fields or via pseudo-magnetic fields generated by intense circularly polarized optical pulses. However, sweeping large magnetic fields is impractical for devices, and the pseudo-magnetic fields are only effective in the presence of ultrafast laser pulses. The recent rise of two-dimensional (2D) magnets unlocks new approaches to control valley physics via van der Waals heterostructure engineering. Here we demonstrate wide continuous tuning of the valley polarization and valley Zeeman splitting with small changes in the laser excitation power in heterostructures formed by monolayer WSe$_2$ and 2D magnetic chromium triiodide (CrI$_3$). The valley manipulation is realized via optical control of the CrI$_3$magnetization, which tunes the magnetic exchange field over a range of 20 T. Our results reveal a convenient new path towards optical control of valley pseudospins and van der Waals magnetic heterostructures., Comment: 10 pages main text, 4 figures, 12 pages supplementary information, in Nano Letters

Efficient coupling between on-chip sources and cavities plays a key role in silicon photonics. However, despite the importance of this basic functionality, there are few systematic design tools to simultaneously control coupling between multiple modes in a compact resonator and a single waveguide. Here, we propose a large-scale adjoint optimization approach to produce wavelength-scale waveguide--cavity couplers operating over tunable and broad frequency bands. We numerically demonstrate couplers discovered by this method that can achieve critical, or nearly critical, coupling between multi-ring cavities and a single waveguide at up to six widely separated wavelengths spanning the $560$--$1500$~nm range of interest for on-chip nonlinear optical devices., Comment: 5 pages, 3 figures

Generating entangled graph states of qubits requires high entanglement rates, with efficient detection of multiple indistinguishable photons from separate qubits. Integrating defect-based qubits into photonic devices results in an enhanced photon collection efficiency, however, typically at the cost of a reduced defect emission energy homogeneity. Here, we demonstrate that the reduction in defect homogeneity in an integrated device can be partially offset by electric field tuning. Using photonic device-coupled implanted nitrogen vacancy (NV) centers in a GaP-on-diamond platform, we demonstrate large field-dependent tuning ranges and partial stabilization of defect emission energies. These results address some of the challenges of chip-scale entanglement generation.

Defects in crystals are leading candidates for photon-based quantum technologies, but progress in developing practical devices critically depends on improving defect optical and spin properties. Motivated by this need, we study a new defect qubit candidate, the shallow donor in ZnO. We demonstrate all-optical control of the electron spin state of the donor qubits and measure the spin coherence properties. We find a longitudinal relaxation time T$_1$ exceeding 100 ms, an inhomogeneous dephasing time T$_2^*$ of $17\pm2$ ns, and a Hahn spin-echo time T$_2$ of $50\pm13$ $\mu$s. The magnitude of T$_2^*$ is consistent with the inhomogeneity of the nuclear hyperfine field in natural ZnO. Possible mechanisms limiting T$_2$ include instantaneous diffusion and nuclear spin diffusion (spectral diffusion). These results are comparable to the phosphorous donor system in natural silicon, suggesting that with isotope and chemical purification long qubit coherence times can be obtained for donor spins in a direct band gap semiconductor. This work motivates further research on high-purity material growth, quantum device fabrication, and high-fidelity control of the donor:ZnO system for quantum technologies.

The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. Here we create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 photoluminescence intensity strongly depends on the relative alignment between photo-excited spins in WSe2 and the CrI3 magnetization, due to ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure., Comment: Supplementary Materials included. To appear in Science Advances

We perform pulsed optically detected electron spin resonance to measure the DC magnetic field sensitivity and electronic spin coherence time T_2 of an ensemble of near-surface, high-density nitrogen-vacancy (NV) centers engineered to have a narrow magnetic resonance linewidth. Combining pulsed spectroscopy with dynamic nuclear polarization, we obtain the photon-shot-noise-limited DC magnetic sensitivity of 35 nT Hz^{-0.5}. We find that T_2 is controlled by instantaneous diffusion, enabling decoherence spectroscopy on residual nitrogen impurity spins in the diamond lattice and a quantitative determination of their density. The demonstrated high DC magnetic sensitivity and decoherence spectroscopy are expected to broaden the application range for two-dimensional magnetic imaging., Comment: 5 pages, 4 figures

Individual dislocations in an ultra-pure GaAs epilayer are investigated with spatially and spectrally resolved photoluminescence imaging at 5~K. We find that some dislocations act as strong non-radiative recombination centers, while others are efficient radiative recombination centers. We characterize luminescence bands in GaAs due to dislocations, stacking faults, and pairs of stacking faults. These results indicate that low-temperature, spatially-resolved photoluminescence imaging can be a powerful tool for identifying luminescence bands of extended defects. This mapping could then be used to identify extended defects in other GaAs samples solely based on low-temperature photoluminescence spectra., Comment: 4 pages, 4 figures

Scaling beyond two-node quantum networks using nitrogen vacancy (NV) centers in diamond is limited by the low probability of collecting zero phonon line (ZPL) photons from single centers. Here, we demonstrate GaP-on-diamond disk resonators which resonantly couple ZPL photons from single NV centers to single-mode waveguides. In these devices, the probability of a single NV center emitting a ZPL photon into the guided waveguide mode after optical excitation can reach 9%, due to a combination of resonant enhancement of the ZPL emission and efficient coupling between the resonator and waveguide. We verify the single-photon nature of the emission and experimentally demonstrate both high in-waveguide photon numbers and substantial Purcell enhancement for a set of devices. These devices may enable scalable integrated quantum networks based on NV centers., Comment: 8 pages, 6 figures (Including Supplemental Info)

We measure the donor-bound electron longitudinal spin-relaxation time ($T_1$) as a function of magnetic field ($B$) in three high-purity direct-bandgap semiconductors: GaAs, InP, and CdTe, observing a maximum $T_1$ of $1.4~\text{ms}$, $0.4~\text{ms}$ and $1.2~\text{ms}$, respectively. In GaAs and InP at low magnetic field, up to $\sim2~\text{T}$, the spin-relaxation mechanism is strongly density and temperature dependent and is attributed to the random precession of the electron spin in hyperfine fields caused by the lattice nuclear spins. In all three semiconductors at high magnetic field, we observe a power-law dependence ${T_1 \propto B^{-\nu}}$ with ${3\lesssim \nu \lesssim 4}$. Our theory predicts that the direct spin-phonon interaction is important in all three materials in this regime in contrast to quantum dot structures. In addition, the "admixture" mechanism caused by Dresselhaus spin-orbit coupling combined with single-phonon processes has a comparable contribution in GaAs. We find excellent agreement between high-field theory and experiment for GaAs and CdTe with no free parameters, however a significant discrepancy exists for InP., Comment: 20 pages, 12 figures

We present a promising method for creating high-density ensembles of nitrogen-vacancy centers with narrow spin-resonances for high-sensitivity magnetic imaging. Practically, narrow spin-resonance linewidths substantially reduce the optical and RF power requirements for ensemble-based sensing. The method combines isotope purified diamond growth, in situ nitrogen doping, and helium ion implantation to realize a 100 nm-thick sensing surface. The obtained 10^(17) cm^(-3) nitrogen-vacancy density is only a factor of 10 less than the highest densities reported to date, with an observed spin resonance linewidth over 10 times more narrow. The 200 kHz linewidth is most likely limited by dipolar broadening indicating even further reduction of the linewidth is desirable and possible., Comment: 5 pages including references. 3 figures

We investigate the magneto-optical properties of excitons bound to single stacking faults in high-purity GaAs. We find that the two-dimensional stacking fault potential binds an exciton composed of an electron and a heavy-hole, and confirm a vanishing in-plane hole $g$-factor, consistent with the atomic-scale symmetry of the system. The unprecedented homogeneity of the stacking-fault potential leads to ultra-narrow photoluminescence emission lines (with full-width at half maximum ${\lesssim 80~\mu \text{eV} }$) and reveals a large magnetic non-reciprocity effect that originates from the magneto-Stark effect for mobile excitons. These measurements unambiguously determine the direction and magnitude of the giant electric dipole moment (${\gtrsim e \cdot 10~\text{nm}}$) of the stacking-fault exciton, making stacking faults a promising new platform to study interacting excitonic gases., Comment: 5 pages, 3 figures plus supplement

We present chip-scale transmission measurements for three key components of a GaP-on-diamond integrated photonics platform: waveguide-coupled disk resonators, directional couplers, and grating couplers. We also present proof-of-principle measurements demonstrating nitrogen-vacancy (NV) center emission coupled into selected devices. The demonstrated device performance, uniformity and yield place the platform in a strong position to realize measurement-based quantum information protocols utilizing the NV center in diamond., Comment: 8 pages, 8 figures

Excitons in semiconductors can have multiple lifetimes due to spin dependent oscillator strengths and interference between different recombination pathways. In addition, strain and symmetry effects can further modify lifetimes via the removal of degeneracies. We present a convenient formalism for predicting the optical properties of ${k=0}$ excitons with an arbitrary number of charge carriers in different symmetry environments. Using this formalism, we predict three distinct lifetimes for the neutral acceptor bound exciton in GaAs, and confirm this prediction through polarization dependent and time-resolved photoluminescence experiments. We find the acceptor bound-exciton lifetimes to be ${T_o (1,3,3/4)}$ where ${T_o = (0.61 \pm 0.12) \text{ns}}$. Furthermore, we provide an estimate of the intra-level and inter-level exciton spin-relaxation rates., Comment: 5 pages, 3 figures, supplemental information included

Large-scale entanglement of nitrogen-vacancy (NV) centers in diamond will require integration of NV centers with optical networks. Toward this goal, we present the fabrication of single-crystalline gallium phosphide (GaP) resonator-waveguide coupled structures on diamond. We demonstrate coupling between 1 {\mu}m diameter GaP disk resonators and waveguides with a loaded Q factor of 3,800, and evaluate their potential for efficient photon collection if integrated with single photon emitters. This work opens a path toward scalable NV entanglement in the hybrid GaP/diamond platform, with the potential to integrate on-chip photon collection, switching, and detection for applications in quantum information processing., Comment: 9 pages, 5 figures, submitted to Optics Express

Resonantly enhanced emission from the zero phonon line of a diamond nitrogen-vacancy (NV) center in single crystal diamond is demonstrated experimentally using a hybrid whispering gallery mode nanocavity. A 900 nm diameter ring nanocavity formed from gallium phosphide, whose sidewalls extend into a diamond substrate, is tuned onto resonance at low-temperature with the zero phonon line of a negatively charged NV center implanted near the diamond surface. When the nanocavity is on resonance, the zero phonon line intensity is enhanced by approximately an order of magnitude, and the spontaneous emission lifetime of the NV is reduced as much as 18%, corresponding to a 6.3X enhancement of emission in the zero photon line.

We demonstrate coupling of the zero-phonon line of individual nitrogen-vacancy centers and the modes of microring resonators fabricated in single-crystal diamond. A zero-phonon line enhancement exceeding ten-fold is estimated from lifetime measurements at cryogenic temperatures. The devices are fabricated using standard semiconductor techniques and off-the-shelf materials, thus enabling integrated diamond photonics., Comment: 5 pages, 4 figures

The optical transition linewidth and emission polarization of single nitrogen-vacancy (NV) centers are measured from 5 K to room temperature. Inter-excited state population relaxation is shown to broaden the zero-phonon line and both the relaxation and linewidth are found to follow a T^5 dependence for T up to 100 K. This dependence indicates that the dynamic Jahn-Teller effect is the dominant dephasing mechanism for the NV optical transitions at low temperatures.

Optical coupling of nitrogen vacancy centers in single-crystal diamond to an on-chip microcavity is demonstrated. The microcavity is fabricated from a hybrid gallium phosphide and diamond material system, and supports whispering gallery mode resonances with spectrometer resolution limited Q > 25000.

We provide a theoretical framework to study the effect of dephasing on the quantum indistinguishability of single photons emitted from a coherently driven cavity QED $\Lambda$-system. We show that with a large excited-state detuning, the photon indistinguishability can be drastically improved provided that the fluctuation rate of the noise source affecting the excited state is fast compared with the photon emission rate. In some cases a spectral filter is required to realize this improvement, but the cost in efficiency can be made small., Comment: 18 pages, 3 figures, final version

Spin-based quantum computing and magnetic resonance techniques rely on the ability to measure the coherence time, T2, of a spin system. We report on the experimental implementation of all-optical spin echo to determine the T2 time of a semiconductor electron-spin system. We use three ultrafast optical pulses to rotate spins an arbitrary angle and measure an echo signal as the time between pulses is lengthened. Unlike previous spin-echo techniques using microwaves, ultrafast optical pulses allow clean T2 measurements of systems with dephasing times T2* fast in comparison to the timescale for microwave control. This demonstration provides a step toward ultrafast optical dynamic decoupling of spin-based qubits., Comment: 4 pages, 3 figures