Real-time tracking of electron transfer at catalytically active interfaces in lithium-ion batteries.

Transition metals and related compounds are known to exhibit high catalytic activities in various electrochemical reactions thanks to their intriguing electronic structures. What is lesser known is their unique role in storing and transferring electrons in battery electrodes which undergo additional solid-state conversion reactions and exhibit substantially large extra capacities. Here, a full dynamic picture depicting the generation and evolution of electrochemical interfaces in the presence of metallic nanoparticles is revealed in a model CoCO3/Li battery via an in situ magnetometry technique. Beyond the conventional reduction to a Li2CO3/Co mixture under battery operation, further decomposition of Li2CO3 is realized by releasing interfacially stored electrons from its adjacent Co nanoparticles, whose subtle variation in the electronic structure during this charge transfer process has been monitored in real time. The findings in this work may not only inspire future development of advanced electrode materials for next-generation energy storage devices but also open up opportunities in achieving in situ monitoring of important electrocatalytic processes in many energy conversion and storage systems.

Single-domain Bose condensate magnetometer achieves energy resolution per bandwidth below ℏ.

We present a magnetic sensor with energy resolution per bandwidth [Formula: see text] We show how a 87Rb single-domain spinor Bose-Einstein condensate, detected by nondestructive Faraday rotation probing, achieves single-shot low-frequency magnetic sensitivity of 72(8) fT measuring a volume [Formula: see text] for 3.5 s, and thus, [Formula: see text] We measure experimentally the condensate volume, spin coherence time, and readout noise and use phase space methods, backed by three-dimensional mean-field simulations, to compute the spin noise. Contributions to the spin noise include one-body and three-body losses and shearing of the projection noise distribution, due to competition of ferromagnetic contact interactions and quadratic Zeeman shifts. Nonetheless, the fully coherent nature of the single-domain, ultracold two-body interactions allows the system to escape the coherence vs. density trade-off that imposes an energy resolution limit on traditional spin precession sensors. We predict that other Bose-condensed alkalis, especially the antiferromagnetic 23Na, can further improve the energy resolution of this method.

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.

Quantum Gas-Enabled Direct Mapping of Active Current Density in Percolating Networks of Nanowires.

Electrically percolating nanowire networks are among the most promising candidates for next-generation transparent electrodes. Scientific interest in these materials stems from their intrinsic current distribution heterogeneity, leading to phenomena like percolating pathway rerouting and localized self-heating, which can cause irreversible damage. Without an experimental technique to resolve the current distribution and an underpinning nonlinear percolation model, one relies on empirical rules and safety factors to engineer materials. We introduce Bose-Einstein condensate microscopy to address the longstanding problem of imaging active current flow in 2D materials. We report on performance improvement of this technique whereby observation of dynamic redistribution of current pathways becomes feasible. We show how this, combined with existing thermal imaging methods, eliminates the need for assumptions between electrical and thermal properties. This will enable testing and modeling individual junction behavior and hot-spot formation. Investigating both reversible and irreversible mechanisms will contribute to improved performance and reliability of devices.

Magnetoencephalography for Epilepsy Presurgical Evaluation.

PURPOSE OF THE REVIEW: Magnetoencephalography (MEG) is a functional neuroimaging technique that records neurophysiology data with millisecond temporal resolution and localizes it with subcentimeter accuracy. Its capability to provide high resolution in both of these domains makes it a powerful tool both in basic neuroscience as well as clinical applications. In neurology, it has proven useful in its ability to record and localize epileptiform activity. Epilepsy workup typically begins with scalp electroencephalography (EEG), but in many situations, EEG-based localization of the epileptogenic zone is inadequate. The complementary sensitivity of MEG can be crucial in such cases, and MEG has been adopted at many centers as an important resource in building a surgical hypothesis. In this paper, we review recent work evaluating the extent of MEG influence of presurgical evaluations, novel analyses of MEG data employed in surgical workup, and new MEG instrumentation that will likely affect the field of clinical MEG. RECENT FINDINGS: MEG consistently contributes to presurgical evaluation and these contributions often change the plan for epilepsy surgery. Extensive work has been done to develop new analytic methods for localizing the source of epileptiform activity with MEG. Systems using optically pumped magnetometry (OPM) have been successfully deployed to record and localize epileptiform activity. MEG remains an important noninvasive tool for epilepsy presurgical evaluation. Continued improvements in analytic methodology will likely increase the diagnostic yield of the test. Novel instrumentation with OPM may contribute to this as well, and may increase accessibility of MEG by decreasing cost.

A magnon scattering platform.

Scattering experiments have revolutionized our understanding of nature. Examples include the discovery of the nucleus [R. G. Newton, Scattering Theory of Waves and Particles (1982)], crystallography [U. Pietsch, V. Holý, T. Baumback, High-Resolution X-Ray Scattering (2004)], and the discovery of the double-helix structure of DNA [J. D. Watson, F. H. C. Crick, Nature 171, 737-738]. Scattering techniques differ by the type of particles used, the interaction these particles have with target materials, and the range of wavelengths used. Here, we demonstrate a two-dimensional table-top scattering platform for exploring magnetic properties of materials on mesoscopic length scales. Long-lived, coherent magnonic excitations are generated in a thin film of yttrium iron garnet and scattered off a magnetic target deposited on its surface. The scattered waves are then recorded using a scanning nitrogen vacancy center magnetometer that allows subwavelength imaging and operation under conditions ranging from cryogenic to ambient environment. While most scattering platforms measure only the intensity of the scattered waves, our imaging method allows for spatial determination of both amplitude and phase of the scattered waves, thereby allowing for a systematic reconstruction of the target scattering potential. Our experimental results are consistent with theoretical predictions for such a geometry and reveal several unusual features of the magnetic response of the target, including suppression near the target edges and a gradient in the direction perpendicular to the direction of surface wave propagation. Our results establish magnon scattering experiments as a platform for studying correlated many-body systems.

Compact and Fully Integrated LED Quantum Sensor Based on NV Centers in Diamond.

Quantum magnetometry based on optically detected magnetic resonance (ODMR) of nitrogen vacancy centers in diamond nano or microcrystals is a promising technology for sensitive, integrated magnetic-field sensors. Currently, this technology is still cost-intensive and mainly found in research. Here we propose one of the smallest fully integrated quantum sensors to date based on nitrogen vacancy (NV) centers in diamond microcrystals. It is an extremely cost-effective device that integrates a pump light source, photodiode, microwave antenna, filtering and fluorescence detection. Thus, the sensor offers an all-electric interface without the need to adjust or connect optical components. A sensitivity of 28.32nT/Hz and a theoretical shot noise limited sensitivity of 2.87 nT/Hz is reached. Since only generally available parts were used, the sensor can be easily produced in a small series. The form factor of (6.9 × 3.9 × 15.9) mm3 combined with the integration level is the smallest fully integrated NV-based sensor proposed so far. With a power consumption of around 0.1W, this sensor becomes interesting for a wide range of stationary and handheld systems. This development paves the way for the wide usage of quantum magnetometers in non-laboratory environments and technical applications.

Excited-State Lifetime of NV Centers for All-Optical Magnetic Field Sensing.

We investigate the magnetic field-dependent fluorescence lifetime of microdiamond powder containing a high density of nitrogen-vacancy centers. This constitutes a non-intensity quantity for robust, all-optical magnetic field sensing. We propose a fiber-based setup in which the excitation intensity is modulated in a frequency range up to 100MHz. The change in magnitude and phase of the fluorescence relative to B=0 is recorded where the phase shows a maximum in magnetic contrast of 5.8∘ at 13MHz. A lock-in amplifier-based setup utilizing the change in phase at this frequency shows a 100 times higher immunity to fluctuations in the optical path compared to the intensity-based approach. A noise floor of 20µT/Hz and a shot-noise-limited sensitivity of 0.95µT/Hz were determined.

Layer-Dependent Magnetism and Spin Fluctuations in Atomically Thin van der Waals Magnet CrPS4.

van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of the atomically thin vdW magnet chromium thiophosphate CrPS4, revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS4-based spin filter vdW heterostructures. The excellent material stability and robust strategy against environmental degradation in combination with tailored magnetic properties highlight the potential of CrPS4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.

Nanoscale Magnetic Domains in Polycrystalline Mn3Sn Films Imaged by a Scanning Single-Spin Magnetometer.

Noncollinear antiferromagnets with novel magnetic orders, vanishingly small net magnetization, and exotic spin related properties hold enormous promise for developing next-generation, transformative spintronic applications. A major ongoing research focus of this community is to explore, control, and harness unconventional magnetic phases of this emergent material system to deliver state-of-the-art functionalities for modern microelectronics. Here we report direct imaging of magnetic domains of polycrystalline Mn3Sn films, a prototypical noncollinear antiferromagnet, using nitrogen-vacancy-based single-spin scanning microscopy. Nanoscale evolution of local stray field patterns of Mn3Sn samples are systematically investigated in response to external driving forces, revealing the characteristic "heterogeneous" magnetic switching behaviors in polycrystalline textured Mn3Sn films. Our results contribute to a comprehensive understanding of inhomogeneous magnetic orders of noncollinear antiferromagnets, highlighting the potential of nitrogen-vacancy centers to study microscopic spin properties of a broad range of emergent condensed matter systems.

Controlled Surface Modification to Revive Shallow NV- Centers.

Near-surface negatively charged nitrogen vacancy (NV) centers hold excellent promise for nanoscale magnetic imaging and quantum sensing. However, they often experience charge-state instabilities, leading to strongly reduced fluorescence and NV coherence time, which negatively impact magnetic imaging sensitivity. This occurs even more severely at 4 K and ultrahigh vacuum (UHV, p = 2 × 10-10 mbar). We demonstrate that in situ adsorption of H2O on the diamond surface allows the partial recovery of the shallow NV sensors. Combining these with band-bending calculations, we conclude that controlled surface treatments are essential for implementing NV-based quantum sensing protocols under cryogenic UHV conditions.

Application of soil magnetometry and geochemical methods to investigate soil contamination with antimony.

The aim of the study was an assessment of the pollution level and identification of the antimony sources in soils in areas subjected to industrial anthropopressure from: transport, metallurgy and electrical waste recycling. The combination of soil magnetometry, chemical analyzes using atomic spectrometry (ICP-OES and ICP-MS), Sb fractionation analysis, statistical analysis (Pearson's correlation matrix, factor analysis) as well as Geoaccumulation Index, Pollution Load Index, and Sb/As factor allowed not only the assessment of soil contamination degree, but also comprehensive identification of different Sb sources. The results indicate that the soil in the vicinity of the studied objects was characterized by high values of magnetic susceptibility and thus, high contents of potentially toxic elements. The most polluted area was in the vicinity of electrical waste processing plants. Research has shown that the impact of road traffic and wearing off brake blocks, i.e. traffic anthropopression in general, has little effect on the surrounding soil in terms of antimony content. Large amounts of Pb, Zn, As and Cd were found in the soil collected in the vicinity of the heap after the processing of zinc-lead ores, the average antimony (11.31 mg kg-1) content was lower in the vicinity of the heap than in the area around the electrical and electronic waste processing plant, but still very high. Antimony in the studied soils was demobilized and associated mainly with the residual fraction.

Exploring the limits of MEG spatial resolution with multipolar expansions.

The advent of scalp magnetoencephalography (MEG) based on optically pumped magnetometers (OPMs) may represent a step change in the field of human electrophysiology. Compared to cryogenic MEG based on superconducting quantum interference devices (SQUIDs, placed 2-4 cm above scalp), scalp MEG promises significantly higher spatial resolution imaging but it also comes with numerous challenges regarding how to optimally design OPM arrays. In this context, we sought to provide a systematic description of MEG spatial resolution as a function of the number of sensors (allowing comparison of low- vs. high-density MEG), sensor-to-brain distance (cryogenic SQUIDs vs. scalp OPM), sensor type (magnetometers vs. gradiometers; single- vs. multi-component sensors), and signal-to-noise ratio. To that aim, we present an analytical theory based on MEG multipolar expansions that enables, once supplemented with experimental input and simulations, quantitative assessment of the limits of MEG spatial resolution in terms of two qualitatively distinct regimes. In the regime of asymptotically high-density MEG, we provide a mathematically rigorous description of how magnetic field smoothness constraints spatial resolution to a slow, logarithmic divergence. In the opposite regime of low-density MEG, it is sensor density that constraints spatial resolution to a faster increase following a square-root law. The transition between these two regimes controls how MEG spatial resolution saturates as sensors approach sources of neural activity. This two-regime model of MEG spatial resolution integrates known observations (e.g., the difficulty of improving spatial resolution by increasing sensor density, the gain brought by moving sensors on scalp, or the usefulness of multi-component sensors) and gathers them under a unifying theoretical framework that highlights the underlying physics and reveals properties inaccessible to simulations. We propose that this framework may find useful applications to benchmark the design of future OPM-based scalp MEG systems.

Size Selectivity in Heterolanthanide Molecular Complexes with a Ditopic Ligand.

The similar reactivity of lanthanides generally leads to statistically populated polynuclear complexes, making the rational design of ordered hetero-lanthanide compounds extremely challenging. Here we report on the site selectivity in hetero-lanthanide tetranuclear complexes afforded by the relatively simple ditopic pyterpyNO ligand (4'-(4-pyridil)-2,2':6',2"-terpyridine N-oxide). The sequential room temperature reaction of RE2 (tta)6 (pyterpyNO)2 (where RE=Y, (1); Eu, (2), Dy, (3) Htta=2-thenoyltrifluoroacetone) with La(tta)3 dme (dme=dimethoxyethane) yielded Y2 La2 (tta)12 (pyterpyNO)2 (4), Dy2 La2 (tta)12 (pyterpyNO)2 (5) and Eu2 La2 (tta)12 (pyterpyNO)2 (6). Single crystals X-ray diffraction studies showed that 4, 5 and 6 are isostructural, featuring a tetranuclear structure with two different metal coordination sites with coordination numbers 8 (CN8) and 9 (CN9). The two smaller cations are mainly bridged by the O-donor atoms of the NO groups of two pyterpyNO ligands (CN8), while the larger lanthanum centres are bound by a terpyridine unit (CN9). Size selectivity has been studied with structural and magnetic studies in the solid state and through 19 F NMR and photoluminescence studies in solution, showing a direct dependence on the difference of ionic radii of the ions and yielding a 91 % selectivity for 4. Furthermore, 19 F NMR, X-ray and PL studies pointed out that the nature of the product is independent from the synthetic route for compound Eu2 Y2 (tta)12 (pyterpyNO)2 (7), keeping the ion selectivity also for a self-assembly reaction. Unexpectedly, these studies have evidenced that selectivity is not exclusively governed by electrostatic interactions related to size dimensions.

Magnetic nanoparticles in the body parts of Polistes versicolor and Polybia paulista wasps are biomineralized: evidence from magnetization measurements and ferromagnetic resonance spectroscopy.

The detection of the geomagnetic field by animals to use as a cue in homing and migration is known as magnetoreception. The ferromagnetic hypothesis explains magnetoreception assuming that magnetic nanoparticles in cellular structures are used as magnetic field transducers. Considering magnetoreception in social insects, the most studied has been the honeybee Apis mellifera and only in two wasp species (Vespa orientalis and Polybia paulista) have been shown a magnetosensitive behavior. In the present report the body parts (abdomen, head and antennae) of Polistes versicolor and Polybia paulista wasps were studied aiming to find biomineralized magnetic nanoparticles, using magnetometry measurements and ferromagnetic resonance spectroscopy. The magnetometry measurements show the presence of magnetic nanoparticles in all body parts, being characterized as mixtures of superparamagnetic, single domain and pseudo-single domain nanoparticles. From the ferromagnetic resonance spectra were obtained the asymmetry ratio A and the effective g factor geff, and those parameters are consistent with the presence of biomineralized magnetic nanoparticles in both wasps. In the case of Polybia paulista, the magnetic nanoparticles can be associated with some sort of magnetosensor once this wasp is magnetosensitive. For Polistes versicolor, the results indicate that this wasp can be magnetosensitive as Polybia paulista once their magnetic nanoparticles are biomineralized in the body. Behavioral studies with Polistes versicolor wasps deserve to be performed.

Sensitive magnetometry reveals inhomogeneities in charge storage and weak transient internal currents in Li-ion cells.

The ever-increasing demand for high-capacity rechargeable batteries highlights the need for sensitive and accurate diagnostic technology for determining the state of a cell, for identifying and localizing defects, and for sensing capacity loss mechanisms. Here, we leverage atomic magnetometry to map the weak induced magnetic fields around Li-ion battery cells in a magnetically shielded environment. The ability to rapidly measure cells nondestructively allows testing even commercial cells in their actual operating conditions, as a function of state of charge. These measurements provide maps of the magnetic susceptibility of the cell, which follow trends characteristic for the battery materials under study upon discharge. In particular, hot spots of charge storage are identified. In addition, the measurements reveal the capability to measure transient internal current effects, at a level of µA, which are shown to be dependent upon the state of charge. These effects highlight noncontact battery characterization opportunities. The diagnostic power of this technique could be used for the assessment of cells in research, quality control, or during operation, and could help uncover details of charge storage and failure processes in cells.

Automated Machine Learning Strategies for Multi-Parameter Optimisation of a Caesium-Based Portable Zero-Field Magnetometer.

Machine learning (ML) is an effective tool to interrogate complex systems to find optimal parameters more efficiently than through manual methods. This efficiency is particularly important for systems with complex dynamics between multiple parameters and a subsequent high number of parameter configurations, where an exhaustive optimisation search would be impractical. Here we present a number of automated machine learning strategies utilised for optimisation of a single-beam caesium (Cs) spin exchange relaxation free (SERF) optically pumped magnetometer (OPM). The sensitivity of the OPM (T/Hz), is optimised through direct measurement of the noise floor, and indirectly through measurement of the on-resonance demodulated gradient (mV/nT) of the zero-field resonance. Both methods provide a viable strategy for the optimisation of sensitivity through effective control of the OPM's operational parameters. Ultimately, this machine learning approach increased the optimal sensitivity from 500 fT/Hz to <109fT/Hz. The flexibility and efficiency of the ML approaches can be utilised to benchmark SERF OPM sensor hardware improvements, such as cell geometry, alkali species and sensor topologies.

Bayesian-Based Hybrid Method for Rapid Optimization of NV Center Sensors.

NV centers are among the most promising platforms in the field of quantum sensing. Magnetometry based on NV centers, especially, has achieved concrete development in areas of biomedicine and medical diagnostics. Improving the sensitivity of NV center sensors under wide inhomogeneous broadening and fieldamplitude drift is a crucial issue of continuous concern that relies on the coherent control of NV centers with high average fidelity. Quantum optimal control (QOC) methods provide access to this target; nevertheless, the high time consumption of current methods due to the large number of needful sample points as well as the complexity of the parameter space has hindered their usability. In this paper, we propose the Bayesian estimation phase-modulated (B-PM) method to tackle this problem. In the case of the state transforming of an NV center ensemble, the B-PM method reduced the time consumption by more than 90% compared with the conventional standard Fourier basis (SFB) method while increasing the average fidelity from 0.894 to 0.905. In the AC magnetometry scenario, the optimized control pulse obtained with the B-PM method achieved an eight-fold extension of coherence time T2 compared with the rectangular π pulse. Similar application can be made in other sensing situations. As a general algorithm, the B-PM method can be further extended to the open- and closed-loop optimization of complex systems based on a variety of quantum platforms.

Edge-Machine-Learning-Assisted Robust Magnetometer Based on Randomly Oriented NV-Ensembles in Diamond.

Quantum magnetometry based on optically detected magnetic resonance (ODMR) of nitrogen vacancy centers in nano- or micro-diamonds is a promising technology for precise magnetic-field sensors. Here, we propose a new, low-cost and stand-alone sensor setup that employs machine learning on an embedded device, so-called edge machine learning. We train an artificial neural network with data acquired from a continuous-wave ODMR setup and subsequently use this pre-trained network on the sensor device to deduce the magnitude of the magnetic field from recorded ODMR spectra. In our proposed sensor setup, a low-cost and low-power ESP32 microcontroller development board is employed to control data recording and perform inference of the network. In a proof-of-concept study, we show that the setup is capable of measuring magnetic fields with high precision and has the potential to enable robust and accessible sensor applications with a wide measuring range.

Quantum Sensing of Free Radicals in Primary Human Dendritic Cells.

Free radicals are crucial indicators for stress and appear in all kinds of pathogenic conditions, including cancer, cardiovascular diseases, and infection. However, they are difficult to detect due to their reactivity and low abundance. We use relaxometry for the detection of radicals with subcellular resolution. This method is based on a fluorescent defect in a diamond, which changes its optical properties on the basis of the magnetic surroundings. This technique allows nanoscale MRI with unprecedented sensitivity and spatial resolution. Recently, this technique was used inside living cells from a cell line. Cell lines differ in terms of endocytic capability and radical production from primary cells derived from patients. Here we provide the first measurements of phagocytic radical production by the NADPH oxidase (NOX2) in primary dendritic cells from healthy donors. The radical production of these cells differs greatly between donors. We investigated the cell response to stimulation or inhibition.