Imaging the Magnetic Anisotropy in Ultrathin Fe4GeTe2 with a Nitrogen-Vacancy Magnetometer.

Two-dimensional (2D) FenGeTe2, with n = 3, 4, and 5, has been realized in experiments, showing strong magnetic anisotropy with enhanced critical temperature (Tc). The understanding of its magnetic anisotropy is crucial for the exploration of more stable 2D magnets and its spintronic applications. Here, we report a quantitative reconstruction of the magnetization magnitude and its direction in ultrathin Fe4GeTe2 using nitrogen vacancy centers. Through imaging stray magnetic fields, we identified the spin-flop transition at approximately 80 K, resulting in a change of the easy axis from the out-of-plane direction to the in-plane direction. Moreover, by analyzing the thermally activated escape behavior of the magnetization near Tc in terms of the Ginzburg-Landau model, we observed the in-plane magnetic anisotropy effect and the formation capability of magnetic domains at ∼0.4 µm2 µT-1. Our findings contribute to the quantitative understanding of the magnetic anisotropy effect in a vast range of 2D van der Waals magnets.

Single-Shot Readout of a Solid-State Electron Spin Qutrit.

Quantum systems usually feature a rich multilevel structure with promising resources for developing superior quantum technologies compared with their binary counterpart. Single-shot readout of these high-dimensional quantum systems is essential for exploiting their potential. Although there have been various high-spin systems, the single-shot readout of the overall state of high-spin systems remains a challenging issue. Here we demonstrate a reliable single-shot readout of spin qutrit state in a low-temperature solid-state system utilizing a binary readout scheme. We achieve a single-shot readout of an electron spin qutrit associated with a single nitrogen-vacancy center in diamond with an average fidelity of 87.80%. We use this spin qutrit system to verify quantum contextuality, a fundamental test of quantum mechanics. We observe a violation of the noncontextual hidden variable inequality with the developed single-shot readout in contrast to the conventional binary readout. These results pave the way for developing quantum information processing based on spin qutrits.

A convenient and robust design for diamond-based scanning probe microscopes.

Nitrogen-vacancy centers in diamond have been developed as a sensitive magnetic sensor and broadly applied on condensed matter physics. We present a design of a scanning probe microscope based on a nitrogen-vacancy center that can operate under various experimental conditions, including a broad temperature range (20-500 K) and a high-vacuum condition (1 × 10-7 mbar). The design of a compact and robust scanning head and vacuum chamber system is presented, which ensures system stability while enabling the convenience of equipment operations. By showcasing the temperature control performance and presenting confocal images of a single-layer graphene and a diamond probe, along with images of a ferromagnetic strip and an epitaxial BiFeO3 film on the SrTiO3 substrate, we demonstrate the reliability of the instrument. Our study proposes a method and a corresponding design for this microscope that extends its potential applications in nanomagnetism and spintronics.

Sub-nanotesla sensitivity at the nanoscale with a single spin.

High-sensitivity detection of the microscopic magnetic field is essential in many fields. Good sensitivity and high spatial resolution are mutually contradictory in measurement, which is quantified by the energy resolution limit. Here we report that a sensitivity of 0.5 nT/[Formula: see text] at the nanoscale is achieved experimentally by using nitrogen-vacancy defects in diamond with depths of tens of nanometers. The achieved sensitivity is substantially enhanced by integrating with multiple quantum techniques, including real-time-feedback initialization, dynamical decoupling with shaped pulses and repetitive readout via quantum logic. Our magnetic sensors will shed new light on searching new physics beyond the standard model, investigating microscopic magnetic phenomena in condensed matters, and detection of life activities at the sub-cellular scale.

In situ electron paramagnetic resonance spectroscopy using single nanodiamond sensors.

An ultimate goal of electron paramagnetic resonance (EPR) spectroscopy is to analyze molecular dynamics in place where it occurs, such as in a living cell. The nanodiamond (ND) hosting nitrogen-vacancy (NV) centers will be a promising EPR sensor to achieve this goal. However, ND-based EPR spectroscopy remains elusive, due to the challenge of controlling NV centers without well-defined orientations inside a flexible ND. Here, we show a generalized zero-field EPR technique with spectra robust to the sensor's orientation. The key is applying an amplitude modulation on the control field, which generates a series of equidistant Floquet states with energy splitting being the orientation-independent modulation frequency. We acquire the zero-field EPR spectrum of vanadyl ions in aqueous glycerol solution with embedded single NDs, paving the way towards in vivo EPR.

Digital Magnetic Detection of Biomolecular Interactions with Single Nanoparticles.

Biomolecular interactions compose a fundamental element of all life forms and are the biological basis of many biomedical assays. However, current methods for detecting biomolecular interactions have limitations in sensitivity and specificity. Here, using nitrogen-vacancy centers in diamond as quantum sensors, we demonstrate digital magnetic detection of biomolecular interactions with single magnetic nanoparticles (MNPs). We first developed a single-particle magnetic imaging (SiPMI) method on 100 nm-sized MNPs with negligible magnetic background, high signal stability, and accurate quantification. The single-particle method was performed on biotin-streptavidin interactions and DNA-DNA interactions in which a single-base mismatch was specifically differentiated. Subsequently, SARS-CoV-2-related antibodies and nucleic acids were examined by a digital immunomagnetic assay derived from SiPMI. In addition, a magnetic separation process improved the detection sensitivity and dynamic range by more than 3 orders of magnitude and also the specificity. This digital magnetic platform is applicable to extensive biomolecular interaction studies and ultrasensitive biomedical assays.

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.

Self-aligned patterning technique for fabricating high-performance diamond sensor arrays with nanoscale precision.

Efficient, nanoscale precision alignment of defect center creation in photonics structures in challenges the realization of high-performance photonic devices and quantum technology applications. Here, we propose a facile self-aligned patterning technique based on conventional engineering technology, with doping precision that can reach ~15 nm. We demonstrate this technique by fabricating diamond nanopillar sensor arrays with high consistency and near-optimal photon counts. The sensor array achieves high yield approaching the theoretical limit, and high efficiency for filtering sensors with different numbers of nitrogen vacancy centers. Combined with appropriate crystal orientation, the system achieves a saturated fluorescence rate of 4.34 Mcps and effective fluorescence-dependent detection sensitivity of 1800 cps-1/2 . These sensors also show enhanced spin properties in the isotope-enriched diamond. Our technique is applicable to all similar solid-state systems and could facilitate the development of parallel quantum sensing and scalable information processing.

Picotesla magnetometry of microwave fields with diamond sensors.

Developing robust microwave-field sensors is both fundamentally and practically important with a wide range of applications from astronomy to communication engineering. The nitrogen vacancy (NV) center in diamond is an attractive candidate for such purpose because of its magnetometric sensitivity, stability, and compatibility with ambient conditions. However, the existing NV center-based magnetometers have limited sensitivity in the microwave band. Here, we present a continuous heterodyne detection scheme that can enhance the sensor's response to weak microwaves, even in the absence of spin controls. Experimentally, we achieve a sensitivity of 8.9 pT Hz-1/2 for microwaves of 2.9 GHz by simultaneously using an ensemble of nNV ~ 2.8 × 1013 NV centers within a sensor volume of 4 × 10-2 mm3. Besides, we also achieve 1/t scaling of frequency resolution up to measurement time t of 10,000 s. Our scheme removes control pulses and thus will greatly benefit practical applications of diamond-based microwave sensors.

Excited-State Spectroscopy of Spin Defects in Hexagonal Boron Nitride.

A negatively charged boron vacancy (VB-) color center in hexagonal boron nitride has recently been proposed as a promising quantum sensor due to its excellent properties. However, the spin level structure of the VB- color center is still unclear, especially for the excited state. Here we measured and confirmed the excited-state spin transitions of VB- using an optically detected magnetic resonance (ODMR) technique. The zero-field splitting of the excited state is 2.06 GHz, the transverse splitting is 93.1 MHz, and the g factor is 2.04. Moreover, negative peaks in fluorescence intensity and ODMR contrast at the level anticrossing point were observed, and they further confirmed that the spin transitions we measured came from the excited state. Our work deepens the understanding of the excited-state structure of VB- and promotes VB--based quantum sensing applications.

Spin Quantum Heat Engine Quantified by Quantum Steering.

Following the rising interest in quantum information science, the extension of a heat engine to the quantum regime by exploring microscopic quantum systems has seen a boon of interest in the last decade. Although quantum coherence in the quantum system of the working medium has been investigated to play a nontrivial role, a complete understanding of the intrinsic quantum advantage of quantum heat engines remains elusive. We experimentally demonstrate that the quantum correlation between the working medium and the thermal bath is critical for the quantum advantage of a quantum Szilárd engine, where quantum coherence in the working medium is naturally excluded. By quantifying the nonclassical correlation through quantum steering, we reveal that the heat engine is quantum when the demon can truly steer the working medium. The average work obtained by taking different ways of work extraction on the working medium can be used to verify the real quantum Szilárd engine.

Biocompatible Nanotomography of Tightly Focused Light.

Tightly focusing a spatially modulated laser beam lays the foundations for advanced optical techniques, such as a holographic optical tweezer and deterministic super-resolution imaging. Precisely mapping the subwavelength features of those highly confined fields is critical to improving the spatial resolution, especially in highly scattering biotissues. However, current techniques characterizing focal fields are mostly limited to conditions such as under a vacuum and on a glass surface. An optical probe with low cytotoxicity and resistance to autofluorescence is the key to achieving in vivo applications. Here, we use a newly emerging quantum reference beacon, the nitrogen-vacancy (NV) center in the nanodiamond, to characterize the focal field of the near-infrared (NIR) laser focus in Caenorhabditis elegans (C. elegans). This biocompatible background-free focal field mapping technique has the potential to optimize in vivo optical imaging and manipulation.

Immunomagnetic microscopy of tumor tissues using quantum sensors in diamond.

Histological imaging is essential for the biomedical research and clinical diagnosis of human cancer. Although optical microscopy provides a standard method, it is a persistent goal to develop new imaging methods for more precise histological examination. Here, we use nitrogen-vacancy centers in diamond as quantum sensors and demonstrate micrometer-resolution immunomagnetic microscopy (IMM) for human tumor tissues. We immunomagnetically labeled cancer biomarkers in tumor tissues with magnetic nanoparticles and imaged them in a 400-nm resolution diamond-based magnetic microscope. There is barely magnetic background in tissues, and the IMM can resist the impact of a light background. The distribution of biomarkers in the high-contrast magnetic images was reconstructed as that of the magnetic moment of magnetic nanoparticles by employing deep-learning algorithms. In the reconstructed magnetic images, the expression intensity of the biomarkers was quantified with the absolute magnetic signal. The IMM has excellent signal stability, and the magnetic signal in our samples had not changed after more than 1.5 y under ambient conditions. Furthermore, we realized multimodal imaging of tumor tissues by combining IMM with hematoxylin-eosin staining, immunohistochemistry, or immunofluorescence microscopy in the same tissue section. Overall, our study provides a different histological method for both molecular mechanism research and accurate diagnosis of human cancer.

Beating the standard quantum limit under ambient conditions with solid-state spins.

The use of entangled sensors improves the precision limit from the standard quantum limit (SQL) to the Heisenberg limit. Most previous experiments beating the SQL are performed on the sensors that are well isolated under extreme conditions. Here, we demonstrate a sub-SQL interferometer at ambient conditions by using a multispin system, namely, the nitrogen-vacancy (NV) defect in diamond. We achieve two-spin interference with a phase sensitivity of 1.79 ± 0.06 dB beyond the SQL and three-spin interference with a phase sensitivity of 2.77 ± 0.10 dB. Besides, a magnetic sensitivity of 0.87 ± 0.09 dB beyond the SQL is achieved by two-spin interference for detecting a real magnetic field. Particularly, the deterministic and joint initialization of NV negative state, NV electron spin, and two nuclear spins is realized at room temperature. The techniques used here are of fundamental importance for quantum sensing and computing, and naturally applicable to other solid-state spin systems.

Resonant quantum principal component analysis.

Principal component analysis (PCA) has been widely adopted to reduce the dimension of data while preserving the information. The quantum version of PCA (qPCA) can be used to analyze an unknown low-rank density matrix by rapidly revealing the principal components of it, i.e., the eigenvectors of the density matrix with the largest eigenvalues. However, because of the substantial resource requirement, its experimental implementation remains challenging. Here, we develop a resonant analysis algorithm with minimal resource for ancillary qubits, in which only one frequency-scanning probe qubit is required to extract the principal components. In the experiment, we demonstrate the distillation of the first principal component of a 4 × 4 density matrix, with an efficiency of 86.0% and a fidelity of 0.90. This work shows the speedup ability of quantum algorithm in dimension reduction of data and thus could be used as part of quantum artificial intelligence algorithms in the future.

Identity Test of Single NV

Atomiclike defects in solids are not considered to be identical owing to the imperfections of host lattice. Here, we found that even under ambient conditions, negatively charged nitrogen-vacancy (NV^{-}) centers in diamond could still manifest identical at Hz-precision level, corresponding to a 10^{-7}-level relative precision, while the lattice strain can destroy the identity by tens of Hz. All parameters involved in the NV^{-}-^{14}N Hamiltonian are determined by formulating six nuclear frequencies at 10-mHz-level precision and measuring them at Hz-level precision. The most precisely measured parameter, the ^{14}N quadrupole coupling P, is given by -494 575 4.9(8) Hz, whose precision is improved by nearly 4 orders of magnitude compared with previous measurements. We offer an approach for performing precision measurements in solids and deepening our understandings of NV centers as well as other solid-state defects. Besides, these high-precision results imply a potential application of a robust and integrated atomiclike clock based on ensemble NV centers.

A flexible nitrogen-vacancy center probe for scanning magnetometry.

The key component of the scanning magnetometry based on nitrogen-vacancy centers is the diamond probe. Here, we designed and fabricated a new type of probe with an array of pillars on a (100 µm)2 × 50 µm diamond chip. The probe features high yield, convertibility to be a single pillar, and expedient reusability. Our fabrication is dramatically simplified by using ultraviolet laser cutting to shape the chip from a diamond substrate instead of additional lithography and time-consuming reactive ion etching. As an example, we demonstrate the imaging of a single magnetic skyrmion with nanoscale resolution. In the future, this flexible probe will be particularly well-suited for commercial applications.

Parallel optically detected magnetic resonance spectrometer for dozens of single nitrogen-vacancy centers using laser-spot lattice.

We develop a parallel optically detected magnetic resonance (PODMR) spectrometer to address, manipulate, and read out an array of single nitrogen-vacancy (NV) centers in diamond in parallel. In this spectrometer, we use an array of micro-lenses to generate a 20 × 20 laser-spot lattice (LSL) on the objective focal plane and then align the LSL with an array of single NV centers. The quantum states of NV centers are manipulated by a uniform microwave field from a Ω-shape coplanar coil. As an experimental demonstration, we observe 80 NV centers in the field of view. Among them, magnetic resonance (MR) spectra and Rabi oscillations of 18 NV centers along the external magnetic field are measured in parallel. These results can be directly used to realize parallel quantum sensing and multiple times speedup compared with the confocal technique. Regarding the nanoscale MR technique, PODMR will be crucial for a high throughput single molecular MR spectrum and imaging.

Spin-Torque Memristors Based on Perpendicular Magnetic Tunnel Junctions for Neuromorphic Computing.

Spin-torque memristors are proposed in 2009, and can provide fast, low-power, and infinite memristive behavior for neuromorphic computing and large-density non-volatile memory. However, the strict requirements of combining high magnetoresistance, stable domain wall pinning and current-induced switching in a single device pose difficulties in physical implementation. Here, a nanoscale spin-torque memristor based on a perpendicular-anisotropy magnetic tunnel junction with a CoFeB/W/CoFeB composite free layer structure is experimentally demonstrated. Its tunneling magnetoresistance is higher than 200%, and memristive behavior can be realized by spin-transfer torque switching. Memristive states are retained by strong domain wall pinning effects in the free layer. Experiments and simulations suggest that nanoscale vertical chiral spin textures can form around clusters of W atoms under the combined effect of opposite Dzyaloshinskii-Moriya interactions and the Ruderman-Kittel-Kasuya-Yosida interaction between the two CoFeB free layers. Energy fluctuation caused by these textures may be the main reason for the strong pinning effect. With the experimentally demonstrated memristive behavior and spike-timing-dependent plasticity, a spiking neural network to perform handwritten pattern recognition in an unsupervised manner is simulated. Due to advantages such as long endurance and high speed, the spin-torque memristors are competitive in the future applications for neuromorphic computing.

High-fidelity single-shot readout of single electron spin in diamond with spin-to-charge conversion.

High fidelity single-shot readout of qubits is a crucial component for fault-tolerant quantum computing and scalable quantum networks. In recent years, the nitrogen-vacancy (NV) center in diamond has risen as a leading platform for the above applications. The current single-shot readout of the NV electron spin relies on resonance fluorescence method at cryogenic temperature. However, the spin-flip process interrupts the optical cycling transition, therefore, limits the readout fidelity. Here, we introduce a spin-to-charge conversion method assisted by near-infrared (NIR) light to suppress the spin-flip error. This method leverages high spin-selectivity of cryogenic resonance excitation and flexibility of photoionization. We achieve an overall fidelity > 95% for the single-shot readout of an NV center electron spin in the presence of high strain and fast spin-flip process. With further improvements, this technique has the potential to achieve spin readout fidelity exceeding the fault-tolerant threshold, and may also find applications on integrated optoelectronic devices.