De Haas-van Alphen spectroscopy and magnetic breakdown in moiré graphene.

Quantum oscillations originating from the quantization of electron cyclotron orbits provide sensitive diagnostics of electron bands and interactions. We report on nanoscale imaging of the thermodynamic magnetization oscillations caused by the de Haas-van Alphen effect in moiré graphene. Scanning by means of superconducting quantum interference device (SQUID)-on-tip in Bernal bilayer graphene crystal axis-aligned to hexagonal boron nitride reveals large magnetization oscillations with amplitudes reaching 500 Bohr magneton per electron in weak magnetic fields, unexpectedly low frequencies, and high sensitivity to superlattice filling fraction. The oscillations allow us to reconstruct the complex band structure, revealing narrow moiré bands with multiple overlapping Fermi surfaces separated by unusually small momentum gaps. We identified sets of oscillations that violate the textbook Onsager Fermi surface sum rule, signaling formation of broad-band particle-hole superposition states induced by coherent magnetic breakdown.

Imaging quantum oscillations and millitesla pseudomagnetic fields in graphene.

The exceptional control of the electronic energy bands in atomically thin quantum materials has led to the discovery of several emergent phenomena1. However, at present there is no versatile method for mapping the local band structure in advanced two-dimensional materials devices in which the active layer is commonly embedded in the insulating layers and metallic gates. Using a scanning superconducting quantum interference device, here we image the de Haas-van Alphen quantum oscillations in a model system, the Bernal-stacked trilayer graphene with dual gates, which shows several highly tunable bands2-4. By resolving thermodynamic quantum oscillations spanning more than 100 Landau levels in low magnetic fields, we reconstruct the band structure and its evolution with the displacement field with excellent precision and nanoscale spatial resolution. Moreover, by developing Landau-level interferometry, we show shear-strain-induced pseudomagnetic fields and map their spatial dependence. In contrast to artificially induced large strain, which leads to pseudomagnetic fields of hundreds of tesla5-7, we detect naturally occurring pseudomagnetic fields as low as 1 mT corresponding to graphene twisting by 1 millidegree, two orders of magnitude lower than the typical angle disorder in twisted bilayer graphene8-11. This ability to resolve the local band structure and strain at the nanoscale level enables the characterization and use of tunable band engineering in practical van der Waals devices.

Magnetic Imaging and Domain Nucleation in CrSBr Down to the 2D Limit.

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. In this work, 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 evaluation of 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 Néel magnetic domain walls is observed down to the single-layer limit.

Scanning SQUID-on-tip microscope in a top-loading cryogen-free dilution refrigerator.

The scanning superconducting quantum interference device (SQUID) fabricated on the tip of a sharp quartz pipette (SQUID-on-tip) has emerged as a versatile tool for the nanoscale imaging of magnetic, thermal, and transport properties of microscopic devices of quantum materials. We present the design and performance of a scanning SQUID-on-tip microscope in a top-loading probe of a cryogen-free dilution refrigerator. The microscope is enclosed in a custom-made vacuum-tight cell mounted at the bottom of the probe and is suspended by springs to suppress vibrations caused by the pulse tube cryocooler. Two capillaries allow for the in situ control of helium exchange gas pressure in the cell that is required for thermal imaging. A nanoscale heater is used to create local temperature gradients in the sample, which enables quantitative characterization of relative vibrations between the tip and the sample. The spectrum of the vibrations shows distinct resonant peaks with a maximal power density of about 27 nm/Hz1/2 in the in-plane direction. The performance of the SQUID-on-tip microscope is demonstrated by magnetic imaging of the MnBi2Te4 magnetic topological insulator, magnetization and current distribution imaging in a SrRuO3 ferromagnetic oxide thin film, and thermal imaging of dissipation in graphene.

Scanning SQUID microscopy in a cryogen-free cooler.

Scanning superconducting quantum interference device (SQUID) microscopy is a powerful tool for investigating electronic states at surfaces and interfaces by mapping their magnetic signal. SQUID operation requires cryogenic temperatures, which are typically achieved by immersing the cryostat in liquid helium. Making a transition to cryogen free systems is desirable, but has been challenging, as electric noise and vibrations are increased in such systems. We report on the successful operation of a scanning SQUID microscope in a modified Montana Instruments cryogen-free cooler with a base temperature of 4.3 K. We demonstrate scanning SQUID measurements with flux noise performance comparable to a wet system and correlate the sensor-sample vibrations to the cryocooler operation frequencies. In addition, we demonstrate successful operation in a variety of SQUID operation modes, including mapping static magnetic fields, measurement of local susceptibility, and spatial mapping of current flow distribution.

Scanning SQUID susceptometers with sub-micron spatial resolution.

Superconducting QUantum Interference Device (SQUID) microscopy has excellent magnetic field sensitivity, but suffers from modest spatial resolution when compared with other scanning probes. This spatial resolution is determined by both the size of the field sensitive area and the spacing between this area and the sample surface. In this paper we describe scanning SQUID susceptometers that achieve sub-micron spatial resolution while retaining a white noise floor flux sensitivity of ≈2µΦ0/Hz1/2. This high spatial resolution is accomplished by deep sub-micron feature sizes, well shielded pickup loops fabricated using a planarized process, and a deep etch step that minimizes the spacing between the sample surface and the SQUID pickup loop. We describe the design, modeling, fabrication, and testing of these sensors. Although sub-micron spatial resolution has been achieved previously in scanning SQUID sensors, our sensors not only achieve high spatial resolution but also have integrated modulation coils for flux feedback, integrated field coils for susceptibility measurements, and batch processing. They are therefore a generally applicable tool for imaging sample magnetization, currents, and susceptibilities with higher spatial resolution than previous susceptometers.

Electrically Tunable Multiterminal SQUID-on-Tip.

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 pipet 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 µB/Hz1/2 over a continuous field range of 0 to 0.5 T with promising applications for nanoscale scanning magnetic imaging.

Visualization of superparamagnetic dynamics in magnetic topological insulators.

Quantized Hall conductance is a generic feature of two-dimensional electronic systems with broken time reversal symmetry. In the quantum anomalous Hall state recently discovered in magnetic topological insulators, time reversal symmetry is believed to be broken by long-range ferromagnetic order, with quantized resistance observed even at zero external magnetic field. We use scanning nanoSQUID (nano-superconducting quantum interference device) magnetic imaging to provide a direct visualization of the dynamics of the quantum phase transition between the two anomalous Hall plateaus in a Cr-doped (Bi,Sb)2Te3 thin film. Contrary to naive expectations based on macroscopic magnetometry, our measurements reveal a superparamagnetic state formed by weakly interacting magnetic domains with a characteristic size of a few tens of nanometers. The magnetic phase transition occurs through random reversals of these local moments, which drive the electronic Hall plateau transition. Surprisingly, we find that the electronic system can, in turn, drive the dynamics of the magnetic system, revealing a subtle interplay between the two coupled quantum phase transitions.

Three-junction SQUID-on-tip with tunable in-plane and out-of-plane magnetic field sensitivity.

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 µB/Hz(1/2) is demonstrated. This highlights its potential as a local probe of nanoscale magnetic structures.

A scanning superconducting quantum interference device with single electron spin sensitivity.

Superconducting quantum interference devices (SQUIDs) can be used to detect weak magnetic fields and have traditionally been the most sensitive magnetometers available. However, because of their relatively large effective size (on the order of 1 µm), the devices have so far been unable to achieve the level of sensitivity required to detect the field generated by the spin magnetic moment (µB) of a single electron. Here we show that nanoscale SQUIDs with diameters as small as 46 nm can be fabricated on the apex of a sharp tip. The nano-SQUIDs have an extremely low flux noise of 50 nΦ0 Hz(-1/2) and a spin sensitivity of down to 0.38 µB Hz(-1/2), which is almost two orders of magnitude better than previous devices. They can also operate over a wide range of magnetic fields, providing a sensitivity of 0.6 µB Hz(-1/2) at 1 T. The unique geometry of our nano-SQUIDs makes them well suited to scanning probe microscopy, and we use the devices to image vortices in a type II superconductor, spaced 120 nm apart, and to record magnetic fields due to alternating currents down to 50 nT.

Self-aligned nanoscale SQUID on a tip.

A nanometer-sized superconducting quantum interference device (nanoSQUID) is fabricated on the apex of a sharp quartz tip and integrated into a scanning SQUID microscope. A simple self-aligned fabrication method results in nanoSQUIDs with diameters down to 100 nm with no lithographic processing. An aluminum nanoSQUID with an effective area of 0.034 microm2 displays flux sensitivity of 1.8 x 10(-6) Phi(0)/Hz(1/2) and operates in fields as high as 0.6 T. With projected spin sensitivity of 65 micro(B)/Hz(1/2) and high bandwidth, the SQUID on a tip is a highly promising probe for nanoscale magnetic imaging and spectroscopy.

Evidence for a nodal energy gap in the iron-pnictide superconductor LaFePO from penetration depth measurements by scanning SQUID susceptometry.

We measure changes in the penetration depth lambda of the T_{c} approximately 6 K superconductor LaFePO. In the process, scanning SQUID susceptometry is demonstrated as a technique for accurately measuring local temperature-dependent changes in lambda, ideal for studying early or difficult-to-grow materials. lambda is found to vary linearly with temperatures from 0.36 to approximately 2 K, with a slope of 143 +/- 15 A/K, suggesting line nodes in the superconducting order parameter. The linear dependence up to approximately T_{c}/3, similar to the cuprate superconductors, indicates well-developed nodes.

Spinlike susceptibility of metallic and insulating thin films at low temperature.

Susceptibility measurements of patterned thin films at sub-K temperatures were carried out using a scanning SQUID microscope that can resolve signals corresponding to a few hundred Bohr magnetons. Several metallic and insulating thin films, even oxide-free Au films, show a paramagnetic response with a temperature dependence that indicates unpaired spins as the origin. The observed response exhibits a measurable out-of-phase component, which implies that these spins will create 1/f-like magnetic noise. The measured spin density is consistent with recent explanations of low frequency flux noise in SQUIDs and superconducting qubits in terms of spin fluctuations, and suggests that such unexpected spins may be even more ubiquitous than already indicated by earlier measurements. Our measurements set several constraints on the nature of these spins.

Persistent currents in normal metal rings.

The authors have measured the magnetic response of 33 individual cold mesoscopic gold rings, one ring at a time. The response of some sufficiently small rings has a component that is periodic in the flux through the ring and is attributed to a persistent current. Its period is close to h/e, and its sign and amplitude vary between rings. The amplitude distribution agrees well with predictions for the typical h/e current in diffusive rings. The temperature dependence of the amplitude, measured for four rings, is also consistent with theory. These results disagree with previous measurements of three individual metal rings that showed a much larger periodic response than expected. The use of a scanning SQUID microscope enabled in situ measurements of the sensor background. A paramagnetic linear susceptibility and a poorly understood anomaly around a zero field are attributed to defect spins.

Gradiometric micro-SQUID susceptometer for scanning measurements of mesoscopic samples.

We have fabricated and characterized micro-SQUID susceptometers for use in low-temperature scanning probe microscopy systems. The design features the following: a 4.6 mum diameter pickup loop; an integrated field coil to apply a local field to the sample; an additional counterwound pickup-loop/field-coil pair to cancel the background signal from the applied field in the absence of the sample; modulation coils to allow setting the SQUID at its optimum bias point (independent of the applied field), and shielding and symmetry that minimizes coupling of magnetic fields into the leads and body of the SQUID. We use a SQUID series array preamplifier to obtain a system bandwidth of 1 MHz. The flux noise at 125 mK is approximately 0.25 mu Phi 0/ sqrt Hz above 10 kHz, with a value of 2.5 mu Phi 0/ sqrt Hz at 10 Hz. The nominal sensitivity to electron spins located at the center of the pickup loop is approximately 200 muB/ sqrt Hz above 10 kHz, in the white-noise frequency region.

Fluctuation superconductivity in mesoscopic aluminum rings.

Fluctuations are important near phase transitions, where they can be difficult to describe quantitatively. Superconductivity in mesoscopic rings is particularly intriguing because the critical temperature is an oscillatory function of magnetic field. There is an exact theory for thermal fluctuations in one-dimensional superconducting rings, which are therefore expected to be an excellent model system. We measured the susceptibility of many rings, one ring at a time, by using a scanning superconducting quantum interference device that can isolate magnetic signals that are seven orders of magnitude smaller than applied flux. We find that the fluctuation theory describes the results and that a single parameter characterizes the ways in which the fluctuations are especially important at magnetic fields where the critical temperature is suppressed.

Magnetic response of mesoscopic superconducting rings with two order parameters.

The magnetic response and fluxoid transitions of superconducting aluminum rings of various sizes, deposited under conditions likely to generate a layered structure, show good agreement with a two-order-parameter Ginzburg-Landau model. For intermediate couplings, we find metastable states that have different phase winding numbers around the ring in each of the two order parameters. Those states, previously theoretically predicted, are analogous to fractional vortices in singly connected samples with two-order-parameter superconductivity. Larger coupling locks the relative phase so that the two order parameters are only manifest in the temperature dependence of the response. With increasing proximitization, this signature gradually disappears.