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Nano-patterned magnetic materials have opened new venues on the investigation of strongly correlated phenomena including artificial spin-ice systems, geometric frustration, magnetic monopoles, for technologically important applications such as reconfigurable ferromagnetism. With the advent of atomically thin two-dimensional (2D) van der Waals (vdW) magnets a pertinent question is whether such compounds could make their way into this realm where interactions can be tailored so that unconventional states of matter could be assessed. Here we show that square islands of CrGeTe3 vdW ferromagnets distributed in a grid manifest antiferromagnetic correlations, essential to enable frustration resulting in an artificial spin-ice. By using a combination of SQUID-on-tip microscopy, focused ion beam lithography, and atomistic spin dynamic simulations, we show that pristine, isolated CGT flakes as small as 150*150*60 nm3 have tunable dipole-dipole interactions, which can be precisely controlled by their lateral spacing. There is a crossover between non-interacting islands and significant inter-island anticorrelation depending how they are spatially distributed allowing the creation of complex magnetic patterns not observable at the isolated flakes. Our findings suggest that the cross-talk between the nano-patterned magnets can be explored in the generation of even more complex spin configurations where exotic interactions may be manipulated in an unprecedent way., Comment: Main text: 12 pages, 5 figures. Supplementary information: 11 pages, 5 figures

The coercivity of single-domain magnetic nanoparticles typically decreases with the nanoparticle size and reaches zero when thermal fluctuations overcome the magnetic anisotropy. Here, we used SQUID-on-tip microscopy to investigate the coercivity of square-shaped CrGeTe3 nanoislands with a wide range of sizes and width-to-thickness aspect ratios. The results reveal an anomalous size-dependent coercivity, with smaller islands exhibiting higher coercivity. The nonconventional scaling of the coercivity in CrGeTe3 nanoislands was found to be inversely proportional to the island width and thickness (1 over wd). This scaling implies that the nanoisland magnetic anisotropy is proportional to the perimeter rather than the volume, suggesting a magnetic edge state. In addition, we observe that 1600 nm wide islands display multi-domain structures with zero net remnant field, corresponding to the magnetic properties of pristine CrGeTe3 flakes. Our findings highlight the significant influence of edge states on the magnetic properties of CrGeTe3 and deepen our understanding of low-dimensional magnetic systems., Comment: Main text: 11 pages, 3 figures. Supplementary information: 10 pages, 9 figures

Recent advancements in 2D materials have revealed the potential of van der Waals magnets, and specifically of their magnetic anisotropy that allows applications down to the 2D limit. Among these materials, CrSBr has emerged as a promising candidate, because its intriguing magnetic and electronic properties have appeal for both fundamental and applied research in spintronics or magnonics. Here, nano SQUID-on-tip (SOT) microscopy is used to obtain direct magnetic imaging of CrSBr flakes with thicknesses ranging from monolayer (N=1) to few-layer (N=5). The ferromagnetic order is preserved down to the monolayer, while the antiferromagnetic coupling of the layers starts from the bilayer case. For odd layers, at zero applied magnetic field, the stray field resulting from the uncompensated layer is directly imaged. The progressive spin reorientation along the out-of-plane direction (hard axis) is also measured with a finite applied magnetic field, allowing to evaluate the anisotropy constant, which remains stable down to the monolayer and is close to the bulk value. Finally, by selecting the applied magnetic field protocol, the formation of N\'eel magnetic domain walls is observed down to the single layer limit., Comment: Main text: 13 pages, 4 figures. Supplementary information: 10 pages, 7 figures, 1 table

The synthesis of two-dimensional van der Waals magnets has paved the way for both technological applications and fundamental research on magnetism confined to ultra-small length scales. Edge magnetic moments in ferromagnets are expected to be less magnetized than in the sample interior because of the reduced amount of neighboring ferromagnetic spins at the sample edge. We recently demonstrated that CrGeTe3 (CGT) flakes thinner than 10 nm are hard ferromagnets; i.e., they exhibit an open hysteresis loop. In contrast, thicker flakes exhibit zero net remnant field in the interior, with hard ferromagnetism present only at the cleaved edges. This experimental observation suggests that a nontrivial interaction exists between the sample edge and the interior. Here, we demonstrate that artificial edges fabricated by focus ion beam etching also display hard ferromagnetism. This enables us to write magnetic nanowires in CGT directly and use this method to characterize the magnetic interaction between the interior and edge. The results indicate that the interior saturation and depolarization fields depend on the lateral dimensions of the sample. Most notably, the interior region between the edges of a sample narrower than 300 nm becomes a hard ferromagnet, suggesting an enhancement of the magnetic exchange induced by the proximity of the edges. Last, we find that the CGT regions amorphized by the gallium beam are nonmagnetic, which introduces a novel method to tune the local magnetic properties of CGT films, potentially enabling integration into spintronic devices., Comment: Main text: 13 pages, 4 figures. Supplementary information: 8 pages, 6 figures

The interplay between magnetism and superconductivity can lead to unconventional proximity and Josephson effects. A related phenomenon that has recently attracted considerable attention is the superconducting diode effect, in which a non-reciprocal critical current emerges. Although superconducting diodes based on superconducting/ferromagnetic (S/F) bilayers were demonstrated more than a decade ago, the precise underlying mechanism remains unclear. While not formally linked to this effect, the Fulde-Ferrell-Larkin-Ovchinikov (FFLO) state is a plausible mechanism, due to the 2-fold rotational symmetry breaking caused by the finite center-of-mass-momentum of the Cooper pairs. Here, we directly observe, for the first time, a tunable superconducting vortex diode in Nb/EuS (S/F) bilayers. Based on our nanoscale SQUID-on-tip (SOT) microscope and supported by in-situ transport measurements, we propose a theoretical model that captures our key results. Thus, we determine the origin for the vortex diode effect, which builds a foundation for new device concepts.

Abrikosov Vortices have long been considered as means to encode classical information in low-temperature logic circuits (1) and memory devices (2-4). Although it is possible to control individual vortices using local probes (5-11), scalability towards the control of of multiple vortices remains challenging. Vortex logic devices require means to shuttle selected vortices reliably over long distances between engineered pinning potentials. Concomitantly, all other vortices should remains fixed to their precise locations. Here we demonstrate such capabilities using Nb loops patterned below a NbSe$_2$ layer. SQUID-on-Tip (SOT) microscopy reveals that the loops can position vortices in sites designated to a precision better than 100 nm; they can realize "push" and "pull" operations of vortices as far as 3$\mu$m. Successive application of such operations shuttles a vortex between adjacent loops. Our results may be used as means to integrate vortices in future quantum circuitry. Strikingly, we are able to demonstrate a winding operation. Such winding, if realized in topological superconductors, is considered an essential part of future topological quantum information processing (12-17).

CrGeTe3 (CGT) is a semiconducting vdW ferromagnet shown to possess magnetism down to a two-layer thick sample. Although CGT is one of the leading candidates for spintronics devices, a comprehensive analysis of CGT thickness dependent magnetization is currently lacking. In this work, we employ scanning SQUID-on-tip (SOT) microscopy to resolve the magnetic properties of exfoliated CGT flakes at 4.2 K. Combining transport measurements of CGT/NbSe2 samples with SOT images, we present the magnetic texture and hysteretic magnetism of CGT, thereby matching the global behavior of CGT to the domain structure extracted from local SOT magnetic imaging. Using this method, we provide a thickness dependent magnetization state diagram of bare CGT films. No zero-field magnetic memory was found for films thicker than 10 nm and hard ferromagnetism was found below that critical thickness. Using scanning SOT microscopy, we identify a unique edge magnetism, contrasting the results attained in the CGT interior., Comment: Main text: 15 pages, 5 figures. Supplementary information: 9 pages, 10 figures. Supplementary videos: 5

The coupling of a superconductor to a different material often results in a system with unconventional superconducting properties. A conventional superconductor is a perfect diamagnet expelling magnetic fields out of its volume, a phenomenon known as Meissner effect. Here, we show that the simple adsorption of a monolayer of chiral molecules, which are non-magnetic in solution, onto the surface of a conventional superconductor can markedly change its diamagnetic Meissner response. By measuring the internal magnetic field profile in superconducting Nb thin films under an applied transverse field by low-energy muon spin rotation spectroscopy, we demonstrate that the local field profile inside Nb is considerably modified upon molecular adsorption in a way that also depends on the applied field direction. The modification is not limited to the chiral molecules/Nb interface, but it is long ranged and occurs over a length scale comparable to the superconducting coherence length. Zero-field muon spin spectroscopy measurements in combination with our theoretical analysis show that odd-frequency spin-triplet states induced by the chiral molecules are responsible for the modification of the Meissner response observed inside Nb. These results indicate that a chiral molecules/superconductor system supports odd-frequency spin-triplet pairs due to the molecules acting as a spin active layer and therefore they imply that such system can be used as a simpler alternative to superconductor/ferromagnet or superconductor/topological insulator hybrids for the generation and manipulation of unconventional spin-triplet superconducting states., Comment: 13 pages and 5 figures plus Appendixes

Exchange bias is a phenomenon critical to solid-state technologies that require spin valves or non-volatile magnetic memory. The phenomenon is usually studied in the context of magnetic interfaces between antiferromagnets and ferromagnets, where the exchange field of the former acts as a means to pin the polarization of the latter. In the present study, we report an unusual instance of this phenomenon in the topological Weyl semimetal Co3Sn2S2, where the magnetic interfaces associated with domain walls suffice to bias the entire ferromagnetic bulk. Remarkably, our data suggests the presence of a hidden order parameter whose behavior can be independently tuned by applied magnetic fields. For micron-size samples, the domain walls are absent, and the exchange bias vanishes, suggesting the boundaries are a source of pinned uncompensated moment arising from the hidden order. The novelty of this mechanism suggests exciting opportunities lie ahead for the application of topological materials in spintronic technologies., Comment: Main text: 11 pages, 4 figures. Supplementary information: 7 pages, 6 figures. Supplementary videos: 8

A gel consists of a network of particles or molecules formed for example using the sol-gel process, by which a solution transforms into a porous solid. Particles or molecules in a gel are mainly organized on a scaffold that makes up a porous system. Quantized vortices in type II superconductors mostly form spatially homogeneous ordered or amorphous solids. Here we present high-resolution imaging of the vortex lattice displaying dense vortex clusters separated by sparse or entirely vortex-free regions in $\beta$-Bi$_2$Pd superconductor. We find that the intervortex distance diverges upon decreasing the magnetic field and that vortex lattice images follow a multifractal behavior. These properties, characteristic of gels, establish the presence of a novel vortex distribution, distinctly different from the well-studied disordered and glassy phases observed in high-temperature and conventional superconductors. The observed behavior is caused by a scaffold of one-dimensional structural defects with enhanced stress close to the defects. The vortex gel might often occur in type-II superconductors at low magnetic fields. Such vortex distributions should allow to considerably simplify control over vortex positions and manipulation of quantum vortex states.

Quantized magnetic vortices driven by electric current determine key electromagnetic properties of superconductors. While the dynamic behavior of slow vortices has been thoroughly investigated, the physics of ultrafast vortices under strong currents remains largely unexplored. Here we use a nanoscale scanning superconducting quantum interference device to image vortices penetrating into a superconducting Pb film at rates of tens of GHz and moving with velocities up to tens of km/s, which are not only much larger than the speed of sound but also exceed the pair-breaking speed limit of superconducting condensate. These experiments reveal formation of mesoscopic vortex channels which undergo cascades of bifurcations as the current and magnetic field increase. Our numerical simulations predict metamorphosis of fast Abrikosov vortices into mixed Abrikosov-Josephson vortices at even higher velocities. This work offers an insight into the fundamental physics of dynamic vortex states of superconductors at high current densities, crucial for many applications.

Energy dissipation is a fundamental process governing the dynamics of physical, chemical, and biological systems. It is also one of the main characteristics distinguishing quantum and classical phenomena. In condensed matter physics, in particular, scattering mechanisms, loss of quantum information, or breakdown of topological protection are deeply rooted in the intricate details of how and where the dissipation occurs. Despite its vital importance the microscopic behavior of a system is usually not formulated in terms of dissipation because the latter is not a readily measureable quantity on the microscale. Although nanoscale thermometry is gaining much recent interest, the existing thermal imaging methods lack the necessary sensitivity and are unsuitable for low temperature operation required for study of quantum systems. Here we report a superconducting quantum interference nano-thermometer device with sub 50 nm diameter that resides at the apex of a sharp pipette and provides scanning cryogenic thermal sensing with four orders of magnitude improved thermal sensitivity of below 1 {\mu}K/Hz1/2. The non-contact non-invasive thermometry allows thermal imaging of very low nanoscale energy dissipation down to the fundamental Landauer limit of 40 fW for continuous readout of a single qubit at 1 GHz at 4.2 K. These advances enable observation of dissipation due to single electron charging of individual quantum dots in carbon nanotubes and reveal a novel dissipation mechanism due to resonant localized states in hBN encapsulated graphene, opening the door to direct imaging of nanoscale dissipation processes in quantum matter., Comment: Submitted to Nature

We present a new nanoscale superconducting quantum interference device (SQUID) whose interference pattern can be shifted electrically in-situ. The device consists of a nanoscale four-terminal/four-junction SQUID fabricated at the apex of a sharp pipette using a self-aligned three-step deposition of Pb. In contrast to conventional two-terminal/two-junction SQUIDs that display optimal sensitivity when flux biased to about a quarter of the flux quantum, the additional terminals and junctions allow optimal sensitivity at arbitrary applied flux, thus eliminating the magnetic field "blind spots". We demonstrate spin sensitivity of 5 to 8 $\mu_B/\text{Hz}^{1/2}$ over a continuous field range of 0 to 0.5 T, with promising applications for nanoscale scanning magnetic imaging.

Atomically sharp oxide heterostructures exhibit a range of novel physical phenomena that do not occur in the parent bulk compounds. The most prominent example is the appearance of highly conducting and superconducting states at the interface between the band insulators LaAlO3 and SrTiO3. Here we report a new emergent phenomenon at the LaMnO3/SrTiO3 interface in which an antiferromagnetic insulator abruptly transforms into a magnetic state that exhibits unexpected nanoscale superparamagnetic dynamics. Upon increasing the thickness of LaMnO3 above five unit cells, our scanning nanoSQUID-on-tip microscopy shows spontaneous formation of isolated magnetic islands of 10 to 50 nm diameter, which display random moment reversals by thermal activation or in response to an in-plane magnetic field. Our charge reconstruction model of the polar LaMnO3/SrTiO3 heterostructure describes the sharp emergence of thermodynamic phase separation leading to nucleation of metallic ferromagnetic islands in an insulating antiferromagnetic matrix. The model further suggests that the nearby superparamagnetic-ferromagnetic transition can be gate tuned, holding potential for applications in magnetic storage and spintronics.

The dynamics of quantized magnetic vortices and their pinning by materials defects determine electromagnetic properties of superconductors, particularly their ability to carry non-dissipative currents. Despite recent advances in the understanding of the complex physics of vortex matter, the behavior of vortices driven by current through a multi-scale potential of the actual materials defects is still not well understood, mostly due to the scarcity of appropriate experimental tools capable of tracing vortex trajectories on nanometer scales. Using a novel scanning superconducting quantum interference microscope we report here an investigation of controlled dynamics of vortices in lead films with sub-Angstrom spatial resolution and unprecedented sensitivity. We measured, for the first time, the fundamental dependence of the elementary pinning force of multiple defects on the vortex displacement, revealing a far more complex behavior than has previously been recognized, including striking spring softening and broken-spring depinning, as well as spontaneous hysteretic switching between cellular vortex trajectories. Our results indicate the importance of thermal fluctuations even at 4.2 K and of the vital role of ripples in the pinning potential, giving new insights into the mechanisms of magnetic relaxation and electromagnetic response of superconductors., Comment: 15 pages and 5 figures (main text) + 15 pages and 11 figures (supplementary material)

Nanoscale superconducting quantum interference devices (SQUIDs) demonstrate record sensitivities to small magnetic moments, but are typically sensitive only to the field component that is normal to the plane of the SQUID and out-of-plane with respect to the scanned surface. We report on a nanoscale three-junction Pb SQUID which is fabricated on the apex of a sharp tip. Because of its three-dimensional structure, it exhibits a unique tunable sensitivity to both in-plane and out-of-plane fields. We analyze the two-dimensional interference pattern from both numerical and experimental points of view. This device is integrated into a scanning microscope and its ability to independently measure the different components of the magnetic field with outstanding spin sensitivity better than $5\ \frac{\mu_B}{\mathrm{Hz}^{1/2}}$ is demonstrated. This highlights its potential as a local probe of nanoscale magnetic structures.

One of the critical milestones in the intensive pursuit of quantitative nanoscale magnetic imaging tools is achieving the level of sensitivity required for detecting the field generated by the spin magnetic moment {\mu}B of a single electron. Superconducting quantum interference devices (SQUIDs), which were traditionally the most sensitive magnetometers, could not hitherto reach this goal because of their relatively large effective size (of the order of 1 {\mu}m). Here we report self-aligned fabrication of nano-SQUIDs with diameters as small as 46 nm and with an extremely low flux noise of 50 n{\Phi}0/Hz^1/2, representing almost two orders of magnitude improvement in spin sensitivity, down to 0.38 {\mu}B/Hz^1/2. In addition, the devices operate over a wide range of magnetic fields with 0.6 {\mu}B/Hz^1/2 sensitivity even at 1 T. We demonstrate magnetic imaging of vortices in type II superconductor that are 120 nm apart and scanning measurements of AC magnetic fields down to 50 nT. The unique geometry of these nano-SQUIDs that reside on the apex of a sharp tip allows approaching the sample to within a few nm, which paves the way to a new class of single-spin resolved scanning probe microscopy., Comment: 10 pages, 9 figures (including supplementary material), Nature Nanotechnology in press

Fatigue and aging of materials are, in large part, determined by the evolution of the atomic-scale structure in response to strains and perturbations. This coupling between microscopic structure and long time scales remains one of the main challenges in materials study. Focusing on a model system, ion-damaged crystalline silicon, we combine nanocalorimetric experiments with an off-lattice kinetic Monte Carlo simulation to identify the atomistic mechanisms responsible for the structural relaxation over long time scales. We relate the logarithmic relaxation, observed in a number of systems, with heat-release measurements. The microscopic mechanism associated with logarithmic relaxation can be described as a two-step replenish and relax process. As the system relaxes, it reaches deeper energy states with logarithmically growing barriers that need to be unlocked to replenish the heat-releasing events leading to lower energy configurations.