Solid-state Spin Research Articles

All-optical nuclear quantum sensing using nitrogen-vacancy centers in diamond

Solid state spins have demonstrated significant potential in quantum sensing with applications including fundamental science, medical diagnostics and navigation. The quantum sensing schemes showing best performance under ambient conditions all utilize microwave or radio-frequency driving, which poses a significant limitation for miniaturization, energy efficiency, and non-invasiveness of quantum sensors. We overcome this limitation by demonstrating a purely optical approach to coherent quantum sensing. Our scheme involves the 15N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond as a sensing resource, and exploits NV spin dynamics in oblique magnetic fields near the NV’s excited state level anti-crossing to optically pump the nuclear spin into a quantum superposition state. We demonstrate all-optical free-induction decay measurements—the key protocol for low-frequency quantum sensing—both on single spins and spin ensembles. Our results pave the way for highly compact quantum sensors to be employed for magnetometry or gyroscopy applications in challenging environments.

Robustness improvement of a nitrogen-vacancy magnetometer by a double driving method.

The nitrogen vacancy (NV) color center in diamonds is an electron spin that can measure magnetic fields with high sensitivity and resolution. Furthermore, the robustness of an NV-based quantum system should be improved for further application in other sensing methods and in the exploration of basic physics. In this work, the robustness of an NV magnetometer is improved by the double driving method. The sensitivity of the NV magnetometer was improved 2.1 times by strengthening the pumping power from 100 to 600 mW. In this process, thermal drift was introduced, which affects the measurement accuracy. The temperature drift of a diamond matrix was measured using an infrared camera, and the temperature change of a diamond host drifted to ∼80K under high laser and microwave power. To address the drift of temperature owing to sensitivity improvement by pumping enhancement, the double driving method was introduced, to suppress the drift of the resonance frequency, to improve the robustness of a continuous-wave NV magnetometer. The magnetic noise density was improved from 10 to 1.2 nT/Hz1/2. This study checked the source of temperature noise in the process of measuring with the NV color centers and proposes a double driving measurement method to track the resonant frequency change due to environmental temperature drift and improve sensitivity. The findings of this study are useful in applying complex pulse protocols in high-level sensing applications based on solid-state spin.

Properties of Donor Qubits in ZnO Formed by Indium-Ion Implantation

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.

Coherent control of an ultrabright single spin in hexagonal boron nitride at room temperature

Hexagonal boron nitride (hBN) is a remarkable two-dimensional (2D) material that hosts solid-state spins and has great potential to be used in quantum information applications, including quantum networks. However, in this application, both the optical and spin properties are crucial for single spins but have not yet been discovered simultaneously for hBN spins. Here, we realize an efficient method for arraying and isolating the single defects of hBN and use this method to discover a new spin defect with a high probability of 85%. This single defect exhibits outstanding optical properties and an optically controllable spin, as indicated by the observed significant Rabi oscillation and Hahn echo experiments at room temperature. First principles calculations indicate that complexes of carbon and oxygen dopants may be the origin of the single spin defects. This provides a possibility for further addressing spins that can be optically controlled.

On-chip spin-photon entanglement based on photon-scattering of a quantum dot

The realization of on-chip quantum interfaces between flying photons and solid-state spins is a key building block for quantum-information processors, enabling, e.g., distributed quantum computing, where remote quantum registers are interconnected by flying photons. Self-assembled quantum dots integrated into nanostructures are one of the most promising systems for such an endeavor thanks to their near-unity photon-emitter coupling and fast spontaneous emission rate. Here we demonstrate high-fidelity on-chip entanglement between an incoming photon and a stationary quantum-dot hole spin qubit. The entanglement is induced by sequential scattering of the time-bin encoded photon interleaved with active spin control within a microsecond, two orders of magnitude faster than those achieved in other solid-state platforms. Conditioning on the detection of a reflected photon renders the entanglement fidelity immune to the spectral wandering of the emitter. These results represent a major step towards realizing a quantum node capable of interchanging information with flying photons and on-chip quantum logic, as required for quantum networks and quantum repeaters.

Multi-sample/multi-nucleus parallel polarization and monitoring enabled by a fluid path technology compatible cryogenic probe for dissolution dynamic nuclear polarization

Low throughput is one of dissolution Dynamic Nuclear Polarization (dDNP) main shortcomings. Especially for clinical and preclinical applications, where direct 13C nuclei polarization is usually pursued, it takes hours to generate one single hyperpolarized (HP) sample. Being able to hyperpolarize more samples at once represents a clear advantage and can expand the range and complexity of the applications. In this work, we present the design and performance of a highly versatile and customizable dDNP cryogenic probe, herein adapted to a 5 T “wet” preclinical polarizer, that can accommodate up to three samples at once and, most importantly, it is capable of monitoring the solid-state spin dynamics of each sample separately, regardless of the kind of radical used and the nuclear species of interest. Within 30 min, the system was able to dispense three HP solutions with high repeatability across the channels (30.0 ± 1.2% carbon polarization for [1-13C]pyruvic acid doped with trityl radical). Moreover, we tested multi-nucleus NMR capability by polarizing and monitoring simultaneously 13C, 1H and 129Xe. Finally, we implemented [1-13C]lactate/[1-13C]pyruvate polarization and back-to-back dissolution and injection in a healthy mouse model to perform multiple-substrate HP Magnetic Resonance Spectroscopy (MRS) at 14.1 T.

Nuclear spin diffusion under fast magic-angle spinning in solid-state NMR.

Solid-state nuclear spin diffusion is the coherent and reversible process through which spin order is transferred via dipolar couplings. With the recent increases in magic-angle spinning (MAS) frequencies and magnetic fields becoming routinely applied in solid-state nuclear magnetic resonance, understanding how the increased 1H resolution obtained affects spin diffusion is necessary for interpretation of several common experiments. To investigate the coherent contributions to spin diffusion with fast MAS, we have developed a low-order correlation in Liouville space model based on the work of Dumez et al. (J. Chem. Phys. 33, 224501, 2010). Specifically, we introduce a new method for basis set selection, which accounts for the resonance-offset dependence at fast MAS. Furthermore, we consider the necessity of including chemical shift, both isotropic and anisotropic, in the modeling of spin diffusion. Using this model, we explore how different experimental factors change the nature of spin diffusion. Then, we show case studies to exemplify the issues that arise in using spin diffusion techniques at fast spinning. We show that the efficiency of polarization transfer via spin diffusion occurring within a deuterated and 100% back-exchanged protein sample at 60kHz MAS is almost entirely dependent on resonance offset. We additionally identify temperature-dependent magnetization transfer in beta-aspartyl L-alanine, which could be explained by the influence of an incoherent relaxation-based nuclear Overhauser effect.

Robust scheme for high-fidelity generation of mesoscopic entangled cat state

We here study a hybrid quantum system of one solid-state electronic spin coupled to a mechanical resonator (MR) using the crystal strain, with the purpose of engineering the mesoscopic spin-phonon entangled cat state. The feature of this work to be mentioned is that it proposes a different and feasible method to achieve the entanglement, especially with the higher fidelity. This scheme mainly contains two steps, namely the coherent population trapping (CPT) initialization and large-detuning evolution (LDE). By taking all of the adverse decoherence factors into our considerations, the numerical simulations indicate that its fidelity can reach more than 0.995 (or 0.999) when the spin-mechanical coupling strength is 10 (or 100) times larger than spin dephasing and mechanical resonator dissipation rate, respectively. Because of the cooperation of CPT and LDE, this proposal also exhibits a considerable robustness for engineering the entangled cat state, and which may be considered as a general attempt that may be suitable for different systems.

Probing Complex-Energy Topology via Non-Hermitian Absorption Spectroscopy in a Trapped Ion Simulator.

Non-Hermitian systems generically have complex energies, which may host topological structures, such as links or knots. While there has been great progress in experimentally engineering non-Hermitian models in quantum simulators, it remains a significant challenge to experimentally probe complex energies in these systems, thereby making it difficult to directly diagnose complex-energy topology. Here, we experimentally realize a two-band non-Hermitian model with a single trapped ion whose complex eigenenergies exhibit the unlink, unknot, or Hopf link topological structures. Based on non-Hermitian absorption spectroscopy, we couple one system level to an auxiliary level through a laser beam and then experimentally measure the population of the ion on the auxiliary level after a long period of time. Complex eigenenergies are then extracted, illustrating the unlink, unknot, or Hopf link topological structure. Our work demonstrates that complex energies can be experimentally measured in quantum simulators via non-Hermitian absorption spectroscopy, thereby opening the door for exploring various complex-energy properties in non-Hermitian quantum systems, such as trapped ions, cold atoms, superconducting circuits, or solid-state spin systems.

Ferrimagnetic Oscillator Magnetometer

Quantum sensors based on solid-state spins have advanced rapidly over the prior decade, but deploying these sensors in real-world applications remains technically challenging. By introducing an innovative oscillator-based sensor architecture, and employing a ferrimagnetic material rather than the paramagnetic spin defects more commonly studied, this work details the construction of a compact magnetometer with a minimum sensitivity of 100 fT/\ensuremath{\surd}Hz. The sensor's architecture offers advantages in dynamic range, simplicity, and compactness---qualities that may enable widespread use of solid-state quantum sensors outside a laboratory environment.

Characterization and correction of the pulse width effects on quantum sensing experiments using solid-state spin qubits

Pulse-level protocols are commonly used in quantum information and sensing experiments. However, finite pulse width, inevitable in many cases due to experimental conditions, can affect the overall performance of the quantum measurement. Here, we study the effect of finite pulse width on quantum sensing experiments based on the solid-state spin qubits: nitrogen-vacancy centers in diamond. We perform magnetic sensing experiments of DC and AC fields using canonical sensing protocols: Ramsey interferometry, Hahn echo, and XY8 dynamical decoupling. By varying the width of π/2 and π pulse used in the protocols, we estimate the amount of phase accumulation during the pulses and correct their effects by compensating the qubit evolution time for time offsets due to the phase accumulation. In this way, we are able to recover optimal conditions for maximum sensitivity.

High-precision measurements and first-principles explanation of the temperature-dependent C13 and N14 hyperfine interactions of single NV− centers in diamond at room temperature

Revealing the properties of single spin defects in solids is essential for quantum applications based on solid-state systems. However, it is intractable to investigate the temperature-dependent properties of single defects, due to the low precision for single-defect measurements in contrast to defect ensembles. Here we report that the temperature dependence of the Hamiltonian parameters for single negatively charged nitrogen-vacancy centers in diamond at room temperature is precisely measured and the results are in reasonable agreement with first-principles calculations. In particular, the hyperfine interactions with randomly distributed $^{13}\mathrm{C}$ nuclear spins are clearly observed to vary with temperature and the relevant coefficients are measured with hertz-level precision. The temperature-dependent behaviors are attributed to both thermal expansion and lattice vibrations by first-principles calculations. Our results pave the way for taking nuclear spins as more stable thermometers at nanoscale. The methods developed here for high-precision measurements and first-principles calculations can be further extended to other solid-state spin defects.

Robust Quantum Control for the Manipulation of Solid-State Spins

Robust and high-fidelity control of electron spins in solids is the cornerstone for facilitating applications of solid-state spins in quantum information processing and quantum sensing. However, precise control of spin systems is always challenging due to the presence of various noises originating from the thermal environment and control fields. Here, noise-resilient quantum gates, designed with robust optimal control (ROC) algorithms, are demonstrated experimentally with nitrogen-vacancy centers in diamond to realize tailored robustness against detunings and Rabi errors simultaneously. In the presence of both 10% off-resonance detuning and 10% deviation of a Rabi frequency, we achieve an average single-qubit gate fidelity of up to 99.89%. Our experiments also show that, ROC-based multipulse quantum sensing sequences can suppress spurious responses resulting from finite widths and imperfections of microwave pulses, which provides an efficient strategy for enhancing the performance of existing multipulse quantum sensing sequences.

Scalable Quantum Memory Nodes Using Nuclear Spins in Silicon Carbide

A distributed quantum network requires versatile and high-fidelity quantum memory nodes, but it remains challenging to make them scalable. This study investigates the use of multiple controllable quantum memories in silicon carbide---an established semiconductor material platform for various quantum technology applications---and provides a viable solution. The authors show that solid-state spins in silicon carbide are ideal quantum memories in a distributed quantum computing network, wherein a controlled generation of highly coherent qubit registers using nuclear spins is possible. This study will impact the future development of quantum networks with solid states spins as quantum memories.

Single-Spin Readout and Quantum Sensing Using Optomechanically Induced Transparency.

Solid-state spin defects are promising quantum sensors for a large variety of sensing targets. Some of these defects couple appreciably to strain in the host material. We propose to use this strain coupling for mechanically mediated dispersive single-shot spin readout by an optomechanically induced transparency measurement. Surprisingly, the estimated measurement times for negatively charged silicon-vacancy defects in diamond are an order of magnitude shorter than those for single-shot optical fluorescence readout. Our scheme can also be used for general parameter-estimation metrology and offers a higher sensitivity than conventional schemes using continuous position detection.

Coherent optical-microwave interface for manipulation of low-field electronic clock transitions in 171Yb3+:Y2SiO5

The coherent interaction of solid-state spins with both optical and microwave fields provides a platform for a range of quantum technologies, such as quantum sensing, microwave-to-optical quantum transduction and optical quantum memories. Rare-earth ions with electronic spins are interesting in this context. In this work, we use a loop-gap microwave resonator to coherently drive optical and microwave clock transitions simultaneously in a 171Yb3+:Y2SiO5 crystal, achieving a Rabi frequency of 0.56 MHz at 2.497 GHz over a 1-cm long crystal. Furthermore, we provide insights into the spin dephasing at very low fields, showing that superhyperfine-induced collapse of the Hahn echo plays an important role. Our calculations and measurements reveal that the effective magnetic moment can be manipulated in 171Yb3+:Y2SiO5, which suppresses the superhyperfine interaction at the clock transition. At a doping concentration of 2 ppm and 3.4 K, we achieve spin coherence time of 10.0 ± 0.4 ms.

All-Optical Noise Spectroscopy of a Solid-State Spin.

Noise spectroscopy elucidates the fundamental noise sources in spin systems, thereby serving as an essential tool toward developing spin qubits with long coherence times for quantum information processing, communication, and sensing. But existing techniques for noise spectroscopy that rely on microwave fields become infeasible when the microwave power is too weak to generate Rabi rotations of the spin. Here, we demonstrate an alternative all-optical approach to performing noise spectroscopy. Our approach utilizes coherent Raman rotations of the spin state with controlled timing and phase to implement Carr-Purcell-Meiboom-Gill pulse sequences. Analyzing the spin dynamics under these sequences enables us to extract the noise spectrum of a dense ensemble of nuclear spins interacting with a single spin in a quantum dot, which has thus far been modeled only theoretically. By providing spectral bandwidths of over 100 MHz, our approach enables studies of spin dynamics and decoherence for a broad range of solid-state spin qubits.

Enhanced Tripartite Interactions in Spin-Magnon-Mechanical Hybrid Systems.

Coherent tripartite interactions among degrees of freedom of completely different nature are instrumental for quantum information and simulation technologies, but they are generally difficult to realize and remain largely unexplored. Here, we predict a tripartite coupling mechanism in a hybrid setup comprising a single nitrogen-vacancy (NV) center and a micromagnet. We propose to realize direct and strong tripartite interactions among single NV spins, magnons, and phonons via modulating the relative motion between the NV center and the micromagnet. Specifically, by introducing a parametric drive (two-phonon drive) to modulate the mechanical motion (such as the center-of-mass motion of a NV spin in diamond trapped in an electrical trap or a levitated micromagnet in a magnetic trap), we can obtain a tunable and strong spin-magnon-phonon coupling at the single quantum level, with up to 2 orders of magnitude enhancement for the tripartite coupling strength. This enables, for example, tripartite entanglement among solid-state spins, magnons, and mechanical motions in quantum spin-magnonics-mechanics with realistic experimental parameters. This protocol can be readily implemented with the well-developed techniques in ion traps or magnetic traps and could pave the way for general applications in quantum simulations and information processing based on directly and strongly coupled tripartite systems.

Radio-Frequency Electric Field Sensing Based on a Single Solid-State Spin

Nanoscale amplitude and phase sensing of a rf electromagnetic field can benefit broad frontiers in science and technology. The imaging applications in these research areas demand a nanoscale sensor able to detect rf electric fields over a wide frequency range under ambient conditions, which remains a challenge. Here, we present a rf electrometry based on the forbidden magnetic dipole transition of a single shallow nitrogen-vacancy center in diamond and experimentally demonstrate the detection of rf electric fields at frequencies ranging from 13.85 MHz to 2.02 GHz. A sensitivity of $265\phantom{\rule{0.2em}{0ex}}{\mathrm{V}\phantom{\rule{0.2em}{0ex}}\mathrm{cm}}^{\ensuremath{-}1}\phantom{\rule{0.2em}{0ex}}{\mathrm{Hz}}^{\ensuremath{-}1/2}$ for amplitude measurement and a standard deviation of ${0.2}^{\ensuremath{\circ}}$ for phase measurement are achieved. The potential applications of nanoscale sensing and imaging of electromagnetic field are discussed.

99.92%-Fidelity cnot Gates in Solids by Noise Filtering.

Inevitable interactions with the reservoir largely degrade the performance of entangling gates, which hinders practical quantum computation from coming into existence. Here, we experimentally demonstrate a 99.920(7)%-fidelity controlled-not gate by suppressing the complicated noise in a solid-state spin system at room temperature. We found that the fidelity limited at 99% in previous works results from considering only static classical noise, and, thus, in this work, a complete noise model is constructed by also considering the time dependence and the quantum nature of the spin bath. All noises in the model are dynamically corrected by an exquisitely designed shaped pulse, giving the resulting error below 10^{-4}. The residual gate error is mainly originated from the longitudinal relaxation and the waveform distortion that can both be further reduced technically. Our noise-resistant method is universal and will benefit other solid-state spin systems.