Nanoscale Magnetic Imaging Research Articles

Focused electron beam induced deposition of magnetic tips for improved magnetic force microscopy

The combination of focused electron beam induced deposition (FEBID) and magnetic force microscopy (MFM) has opened up new possibilities in nanoscale magnetic imaging. FEBID offers precise control over the dimensions and magnetic properties of the MFM probes, enabling the development of high-performance magnetic tips with enhanced capabilities compared to conventional ones. These improved tips offer superior resolution, sensitivity, and versatility in nanoscale magnetic surface characterization. Here, we compare the performance of a commercial MFM tip and a FEBID-grown Fe tip in a Ni80Fe20/NdCo5 film. The FEBID tip exhibited superior lateral resolution for topography imaging, likely due to its sharper and well-defined geometry, with a tip diameter of approximately 20 nm. MFM measurements further confirmed this advantage, revealing better-defined magnetic domains and higher magnetic contrast with the FEBID-functionalized probes compared to the commercial tip. This improvement can be attributed to the possibility to optimize the tip-sample magnetic interaction for the FEBID tip. By reducing the lift height of the second pass, we were able to bring the tip closer to the sample, enhancing the magnetic signal without introducing significant topographic artifacts. Overall, these findings highlight the potential of FEBID for creating high-resolution and high-sensitivity MFM tips.

Super-Resolution Diamond Magnetic Microscopy of Superparamagnetic Nanoparticles.

Scanning-probe and wide-field magnetic microscopes based on nitrogen-vacancy (NV) centers in diamond have enabled advances in the study of biology and materials, but each method has drawbacks. Here, we implement an alternative method for nanoscale magnetic microscopy based on optical control of the charge state of NV centers in a dense layer near the diamond surface. By combining a donut-beam super-resolution technique with optically detected magnetic resonance spectroscopy, we imaged the magnetic fields produced by single 30 nm iron-oxide nanoparticles. The magnetic microscope has a lateral spatial resolution of ∼100 nm, and it resolves the individual magnetic dipole features from clusters of nanoparticles with interparticle spacings down to ∼190 nm. The magnetic feature amplitudes are more than an order of magnitude larger than those obtained by confocal magnetic microscopy due to the narrower optical point-spread function and the shallow depth of NV centers. We analyze the magnetic nanoparticle images and sensitivity as a function of the microscope's spatial resolution and show that the signal-to-noise ratio for nanoparticle detection does not degrade as the spatial resolution improves. We identify sources of background fluorescence that limit the present performance, including diamond second-order Raman emission and imperfect NV charge state control. Our method, which uses <10 mW laser power and can be parallelized by patterned illumination, introduces a promising format for nanoscale magnetic imaging.

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.

Magnetic force microscopy of an operational spin nano-oscillator

Magnetic force microscopy (MFM) is a powerful technique for studying magnetic microstructures and nanostructures that relies on force detection by a cantilever with a magnetic tip. The detected magnetic tip interactions are used to reconstruct the magnetic structure of the sample surface. Here, we demonstrate a new method using MFM for probing the spatial profile of an operational nanoscale spintronic device, the spin Hall nano-oscillator (SHNO), which generates high-intensity spin wave auto-oscillations enabling novel microwave applications in magnonics and neuromorphic computing. We developed an MFM system by adding a microwave probe station to allow electrical and microwave characterization up to 40 GHz during the MFM process. SHNOs—based on NiFe/Pt bilayers with a specific design compatible with the developed system—were fabricated and scanned using a Co magnetic force microscopy tip with 10 nm spatial MFM resolution, while a DC current sufficient to induce auto-oscillation flowed. Our results show that this developed method provides a promising path for the characterization and nanoscale magnetic field imaging of operational nano-oscillators.

Proximal nitrogen reduces the fluorescence quantum yield of nitrogen-vacancy centres in diamond

The nitrogen-vacancy colour centre in diamond is emerging as one of the most important solid-state quantum systems. It has applications to fields including high-precision sensing, quantum computing, single photon communication, metrology, nanoscale magnetic imaging and biosensing. For all of these applications, a high quantum yield of emitted photons is desirable. However, diamond samples engineered to have high densities of nitrogen-vacancy centres show levels of brightness varying significantly within single batches, or even within the same sample. Here we show that nearby nitrogen impurities quench emission of nitrogen-vacancy centres via non-radiative transitions, resulting in a reduced fluorescence quantum yield. We monitored the emission properties of nitrogen-vacancy centre ensembles from synthetic diamond samples with different concentrations of nitrogen impurities. All samples were irradiated with high energy electrons to create high densities of nitrogen-vacancy centres relative to the concentration of nitrogen impurities. While at low nitrogen densities of 1.81 ppm we measured a lifetime of 13.9 ns, we observed a strong reduction in lifetime with increasing nitrogen density. We measure a lifetime as low as 4.4 ns at a nitrogen density of 380 ppm. The change in lifetime matches a reduction in relative fluorescence quantum yield from 77.4% to 32% with an increase in nitrogen density from 88 ppm to 380 ppm, respectively. These results will inform the conditions required to optimise the properties of diamond crystals devices based on the fluorescence of nitrogen-vacancy centres. Furthermore, this work provides insights into the origin of inhomogeneities observed in high-density nitrogen-vacancy ensembles within diamonds and nanodiamonds.

Nanoscale magnetic field imaging for 2D materials

Nanometer-scale imaging of magnetization and current density is the key to deciphering the mechanisms behind a variety of new and poorly understood condensed matter phenomena. The recently discovered correlated states hosted in atomically layered materials such as twisted bilayer graphene or van der Waals heterostructures are noteworthy examples. Manifestations of these states range from superconductivity, to highly insulating states, to magnetism. Their fragility and susceptibility to spatial inhomogeneities limits their macroscopic manifestation and complicates conventional transport or magnetization measurements, which integrate over an entire sample. In contrast, techniques for imaging weak magnetic field patterns with high spatial resolution overcome inhomogeneity by measuring the local fields produced by magnetization and current density. Already, such imaging techniques have shown the vulnerability of correlated states in twisted bilayer graphene to twist-angle disorder and revealed the complex current flows in quantum Hall edge states. Here, we review the state-of-the-art techniques most amenable to the investigation of such systems, because they combine the highest magnetic field sensitivity with the highest spatial resolution and are minimally invasive: magnetic force microscopy, scanning superconducting quantum interference device microscopy, and scanning nitrogen-vacancy center microscopy. We compare the capabilities of these techniques, their required operating conditions, and assess their suitability to different types of source contrast, in particular magnetization and current density. Finally, we focus on the prospects for improving each technique and speculate on its potential impact, especially in the rapidly growing field of two-dimensional (2D) materials.

Multiangle Reconstruction of Domain Morphology with All-Optical Diamond Magnetometry

Scanning diamond magnetometers based on the optically detected magnetic resonance of the nitrogen-vacancy centre offer very high sensitivity and non-invasive imaging capabilities when the stray fields emanating from ultrathin magnetic materials are sufficiently low (< 10 mT). Beyond this low-field regime, the optical signal quenches and a quantitative measurement is challenging. While the field-dependent NV photoluminescence can still provide qualitative information on magnetic morphology, this operation regime remains unexplored particularly for surface magnetisation larger than $\sim$ 3 mA. Here, we introduce a multi-angle reconstruction technique (MARe) that captures the full nanoscale domain morphology in all magnetic-field regimes leading to NV photoluminescence quench. To demonstrate this, we use [Ir/Co/Pt]$_{14}$ multilayer films with surface magnetisation an order of magnitude larger than previous reports. Our approach brings non-invasive nanoscale magnetic field imaging capability to the study of a wider pool of magnetic materials and phenomena.

Parabolic Diamond Scanning Probes for Single-Spin Magnetic Field Imaging

Enhancing the measurement signal from solid state quantum sensors such as the nitrogen-vacancy (NV) center in diamond is an important problem for sensing and imaging of condensed matter systems. Here we engineer diamond scanning probes with a truncated parabolic profile that optimizes the photonic signal from single embedded NV centers, forming a high-sensitivity probe for nanoscale magnetic field imaging. We develop a scalable fabrication procedure based on dry etching with a flowable oxide mask to reliably produce a controlled tip curvature. The resulting parabolic tip shape yields a median saturation count rate of 2.1 $\pm$ 0.2 MHz, the highest reported for single NVs in scanning probes to date. Furthermore, the structures operate across the full NV photoluminescence spectrum, emitting into a numerical aperture of 0.46 and the end-facet of the truncated tip, located near the focus of the parabola, allows for small NV-sample spacings and nanoscale imaging. We demonstrate the excellent properties of these diamond scanning probes by imaging ferromagnetic stripes with a spatial resolution better than 50 nm. Our results mark a 5-fold improvement in measurement signal over the state-of-the art in scanning-probe based NV sensors.

Imaging viscous flow of the Dirac fluid in graphene

The electron-hole plasma in charge-neutral graphene is predicted to realize a quantum critical system in which electrical transport features a universal hydrodynamic description, even at room temperature1,2. This quantum critical 'Dirac fluid' is expected to have a shear viscosity close to a minimum bound3,4, with an interparticle scattering rate saturating1 at the Planckian time,the shortest possible timescale for particles to relax. Although electrical transport measurements at finite carrier density are consistent with hydrodynamic electron flow in graphene5-8, a clear demonstration of viscous flow at the charge-neutrality point remains elusive. Here we directly image viscous Dirac fluid flow in graphene at room temperature by measuring the associated stray magnetic field. Nanoscale magnetic imaging is performed using quantum spin magnetometers realized with nitrogen vacancy centres in diamond. Scanning single-spin and wide-field magnetometry reveal a parabolic Poiseuille profile for electron flow in a high-mobility graphene channel near the charge-neutrality point, establishing the viscous transport of the Dirac fluid. This measurement is in contrast to the conventional uniform flow profile imaged in a metallic conductor and also in a low-mobility graphene channel. Via combined imaging and transport measurements, we obtain viscosity and scattering rates, and observe that these quantities are comparable to the universal values expected at quantum criticality. This finding establishes a nearly ideal electron fluid in charge-neutral, high-mobility graphene at room temperature4. Our results will enable the study of hydrodynamic transport in quantum critical fluids relevant to strongly correlated electrons in high-temperature superconductors9. This work also highlights the capability of quantum spin magnetometers to probe correlated electronic phenomena at the nanoscale.

Nanoscale magnetic imaging enabled by nitrogen vacancy centres in nanodiamonds labelled by iron-oxide nanoparticles.

Nanodiamonds containing the nitrogen vacancy centre (NV) have a significant role in biosensing, bioimaging, drug delivery, and as biomarkers in fluorescence imaging, due to their photo-stability and biocompatibility. The optical read out of the NV unpaired electron spin has been used in diamond magnetometry to image living cells and magnetically labelled cells. Diamond magnetometry is mostly based on the use of bulk diamond with a large concentration of NV centres in a wide field fluorescence microscope equipped with microwave excitation. It is possible to correlate the fluorescence maps with the magnetic field maps of magnetically labelled cells with diffraction limit resolution. Nanodiamonds have not as yet been implemented to image magnetic fields within complex biological systems at the nanometre scale. Here we demonstrate the suitability of nanodiamonds to correlate the fluorescence map with the magnetic imaging map of magnetically labelled cells. Nanoscale optical images with 17 nm resolution of nanodiamonds labelling fixed cells bound to iron oxide magnetic nanoparticles are demonstrated by using a single molecule localisation microscope. Nanoscale magnetic field images of the magnetised magnetic nanoparticles spatially assigned to individual cells are superresolved by the NV centres within nanodiamonds conjugated with the magnetic nanoparticles with 20 nm resolutions. Our method offers a new platform for the super-resolution of optical magnetic imaging in biological samples conjugated with nanodiamonds and iron-oxide magnetic nanoparticles.

Nanoscale graphene Hall sensors for high-resolution ambient magnetic imaging

A major challenge to routine non-invasive, nanoscale magnetic imaging is the development of Hall sensors that are stable under ambient conditions and retain low minimum detectable fields down to nanoscale dimensions. To address these issues we have fabricated and characterised chemical vapour deposition (CVD) graphene Hall sensors with wire widths between 50 nm and 1500 nm, in order to exploit the high carrier mobility and tuneability of this material. The measured Hall voltage noise is in good agreement with theoretical models and we demonstrate that minimum detectable fields at fixed drive current are lowest in the vicinity of the charge neutrality point. Our best performing deep sub-micron sensors, based on a wire width of 85 nm, display the excellent room temperature resolution of 59 µT/√Hz at a dc drive current of 12 µA and measurement frequency of 531 Hz. We observe a weak increase in minimum detectable field as the active sensor area is reduced while the Hall offset field is largely independent of size. These figures-of-merit significantly surpass prior results on larger probes in competing materials systems, with considerable scope for further optimisation. Our results clearly demonstrate the feasibility of using CVD graphene to realise very high spatial resolution nanosensors for quantitative room temperature magnetic imaging.

Nanoscale magnetic imaging of ferritins in a single cell.

The in situ measurement of the distribution of biomolecules inside a cell is one of the important goals in life science. Among various imaging techniques, magnetic imaging (MI) based on the nitrogen-vacancy (NV) center in diamond provides a powerful tool for the biomolecular research, while the nanometer-scale MI of intracellular proteins remains a challenge. Here, we use ferritin as a demonstration to realize the MI of endogenous proteins in a single cell using the NV center as the sensor. With the scanning, intracellular ferritins are imaged with a spatial resolution of ca. 10 nm, and ferritin-containing organelles are colocalized by correlative MI and electron microscopy. The approach paves the way for nanoscale MI of intracellular proteins.

Dynamics of the Bloch point in an asymmetric permalloy disk

A Bloch point (BP) is a topological defect in a ferromagnet at which the local magnetization vanishes. With the difficulty of generating a stable BP in magnetic nanostructures, the intrinsic nature of a BP and its dynamic behaviour has not been verified experimentally. We report a realization of steady-state BPs embedded in deformed magnetic vortex cores in asymmetrically shaped Ni80Fe20 nanodisks. Time-resolved nanoscale magnetic X-ray imaging combined with micromagnetic simulation shows detailed dynamic character of BPs, revealing rigid and limited lateral movements under magnetic field pulses as well as its crucial role in vortex-core dynamics. Direct visualizations of magnetic structures disclose the unique dynamical feature of a BP as an atomic scale discrete spin texture and allude its influence on the neighbouring spin structures such as magnetic vortices.

Realisation of a frustrated 3D magnetic nanowire lattice

Patterning nanomagnets in three-dimensions presents a new paradigm in condensed matter physics and allows access to a plethora of phenomena including robust spin textures, magnetic metamaterials home to defects carrying magnetic charge and ultrahigh density devices that store information in three-dimensions. However, the nanostructuring of functional magnetic materials into complex three-dimensional geometries has thus far proven to be a formidable challenge. Here we show magnetic nanowires can be arranged into 3D frustrated magnetic nanowire lattices by using a combination of 3D polymer nanoprinting and metallic deposition. The fabricated nanowires are single domain and they switch via nucleation and propagation of domain walls. Deep nanoscale magnetic imaging and finite element simulations elucidate the spin texture present on the 3D nanostructured lattice. Our study demonstrates a generic platform for the production of 3D nanostructured magnetic materials allowing the realisation of racetrack memory devices and 3D nanostructured systems that mimic bulk frustrated crystals.

Nanoscale magnetic imaging using circularly polarized high-harmonic radiation.

This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the exceptional coherence of high harmonics, this approach will facilitate quantitative, element-specific, and spatially resolved studies of ultrafast magnetization dynamics, advancing both fundamental and applied aspects of nanoscale magnetism.

Quantitative nanoscale vortex imaging using a cryogenic quantum magnetometer.

Microscopic studies of superconductors and their vortices play a pivotal role in understanding the mechanisms underlying superconductivity. Local measurements of penetration depths or magnetic stray fields enable access to fundamental aspects such as nanoscale variations in superfluid densities or the order parameter symmetry of superconductors. However, experimental tools that offer quantitative, nanoscale magnetometry and operate over large ranges of temperature and magnetic fields are still lacking. Here, we demonstrate the first operation of a cryogenic scanning quantum sensor in the form of a single nitrogen-vacancy electronic spin in diamond, which is capable of overcoming these existing limitations. To demonstrate the power of our approach, we perform quantitative, nanoscale magnetic imaging of Pearl vortices in the cuprate superconductor YBa2Cu3O7-δ. With a sensor-to-sample distance of ∼10 nm, we observe striking deviations from the prevalent monopole approximation in our vortex stray-field images, and find excellent quantitative agreement with Pearl's analytic model. Our experiments provide a non-invasive and unambiguous determination of the system's local penetration depth and are readily extended to higher temperatures and magnetic fields. These results demonstrate the potential of quantitative quantum sensors in benchmarking microscopic models of complex electronic systems and open the door for further exploration of strongly correlated electron physics using scanning nitrogen-vacancy magnetometry.

Polarization contrast of nanoscale waveguides in high harmonic imaging

The optical polarization response of a structured material is one of its most significant properties, carrying information about microscopic anisotropies as well as chiral features and spin orientations. Polarization analysis is therefore a key element of imaging and spectroscopy techniques throughout the entire spectrum. In the case of extreme ultraviolet (EUV) radiation, however, both the preparation and detection of well-defined polarization states remain challenging. As a result, polarization-sensitive EUV microscopy based on table-top sources has not yet been realized, despite its great potential, for example, in nanoscale magnetic imaging. Here, we demonstrate polarization contrast in coherent diffractive imaging using high harmonic radiation and investigate the polarization properties of nanoscale transmission waveguides. We quantify the achievable polarization extinction ratio for different waveguide geometries and wavelengths. Our results demonstrate the utility of slab waveguides for efficient EUV polarization control and illustrate the importance of considering polarization contrast in the imaging of nanoscale structures.

Scanning Nanospin Ensemble Microscope for Nanoscale Magnetic and Thermal Imaging.

Quantum sensors based on solid-state spins provide tremendous opportunities in a wide range of fields from basic physics and chemistry to biomedical imaging. However, integrating them into a scanning probe microscope to enable practical, nanoscale quantum imaging is a highly challenging task. Recently, the use of single spins in diamond in conjunction with atomic force microscopy techniques has allowed significant progress toward this goal, but generalization of this approach has so far been impeded by long acquisition times or by the absence of simultaneous topographic information. Here, we report on a scanning quantum probe microscope which solves both issues by employing a nanospin ensemble hosted in a nanodiamond. This approach provides up to an order of magnitude gain in acquisition time while preserving sub-100 nm spatial resolution both for the quantum sensor and topographic images. We demonstrate two applications of this microscope. We first image nanoscale clusters of maghemite particles through both spin resonance spectroscopy and spin relaxometry, under ambient conditions. Our images reveal fast magnetic field fluctuations in addition to a static component, indicating the presence of both superparamagnetic and ferromagnetic particles. We next demonstrate a new imaging modality where the nanospin ensemble is used as a thermometer. We use this technique to map the photoinduced heating generated by laser irradiation of a single gold nanoparticle in a fluid environment. This work paves the way toward new applications of quantum probe microscopy such as thermal/magnetic imaging of operating microelectronic devices and magnetic detection of ion channels in cell membranes.

Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond.

Optically detected magnetic resonance using nitrogen-vacancy (NV) colour centres in diamond is a leading modality for nanoscale magnetic field imaging, as it provides single electron spin sensitivity, three-dimensional resolution better than 1 nm (ref. 5) and applicability to a wide range of physical and biological samples under ambient conditions. To date, however, NV-diamond magnetic imaging has been performed using 'real-space' techniques, which are either limited by optical diffraction to ∼250 nm resolution or require slow, point-by-point scanning for nanoscale resolution, for example, using an atomic force microscope, magnetic tip, or super-resolution optical imaging. Here, we introduce an alternative technique of Fourier magnetic imaging using NV-diamond. In analogy with conventional magnetic resonance imaging (MRI), we employ pulsed magnetic field gradients to phase-encode spatial information on NV electronic spins in wavenumber or 'k-space' followed by a fast Fourier transform to yield real-space images with nanoscale resolution, wide field of view and compressed sensing speed-up.

Atomic-Scale Nuclear Spin Imaging Using Quantum-Assisted Sensors in Diamond

Manufacturing potent drugs requires knowledge of protein receptor sites. A novel strategy, combining the use of a quantum memory with quantum control, can boost the spatial resolution of magnetic-field sensors based on spin defects in diamond, thus achieving nanoscale magnetic imaging of biomolecules.