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We have characterised the submonolayer assembly of C60F48 molecular surface acceptors on the hydrogen terminated (100) diamond surface using scanning tunneling microscopy and X-ray photoelectron spectroscopy, and explored the influence this assembly has on the energy level alignment which governs surface transfer doping. Following deposition, disordered multilayered islands are observed. Annealing to 90$^{\circ} \rm{C}$ causes a transition from dewetting multi-layered islands to a single wetting layer at sufficiently high coverage, accompanied by a change in the energy alignment between the C60F48 and the diamond surface which consequently decreased the carrier density induced by transfer doping by 20%., Comment: 13 pages, 10 figures, preprint

The kagome metal FeSn, consists of alternating layers of kagome-lattice Fe3Sn and honeycomb Sn2, and exhibits great potential for applications in future low energy electronics and spintronics because of an ideal combination of novel topological phases and high-temperature magnetic ordering. Robust synthesis methods for ultra-thin FeSn films, as well as an understanding of their air stability is crucial for its development and long-term operation in future devices. In this work, we realize large area, sub-10 nm epitaxial FeSn thin films, and explore the oxidation process via synchrotron-based photoelectron spectroscopy using in-situ oxygen and water dosing, as well as ex-situ air exposure. Upon exposure to atmosphere the FeSn films are shown to be highly reactive, with a stable ~3 nm thick oxide layer forming at the surface within 10 minutes. Notably the surface Fe remains largely unoxidized when compared to Sn, which undergoes near-complete oxidation. This is further confirmed with controlled in-situ dosing of O2 and H2O where only the Sn2 (stanene) inter-layers within the FeSn lattice oxidize, suggesting the Fe3Sn kagome layers remain almost pristine. These results are in excellent agreement with first principles calculations, which show Fe-O bonds to the Fe3Sn layer are energetically unfavorable, and furthermore, a large formation energy preference of 1.37 eV for Sn-O bonds in the stanene Sn2 layer over Sn-O bonds in the kagome Fe3Sn layer. The demonstration that oxidation only occurs within the stanene layers may provide new avenues in how to engineer, handle and prepare future kagome metal devices., Comment: 21 pages, 5 figures, 4 SI figures

Topological insulators (TIs) are emergent materials with unique band structure, which allow the study of quantum effect in solids, as well as contribute to high performance quantum devices. To achieve the better performance of TI, here we present a co-doping strategy using synergistic rare-earth Sm and transition-metal Fe dopants in Bi2Se3 single crystals, which combine the advantages of both transition metal doped TI (high ferromagnetic ordering temperature and observed QAHE), and rare-earth doped TI (large magnetic moments and significant spin orbit coupling). In the as-grown single crystals, clear evidences of ferromagnetic ordering were observed. The angle resolve photoemission spectroscopy indicate the ferromagnetism opens a 44 meV band gap at surface Dirac point. Moreover, the carrier mobility at 3 K is ~ 7400 cm2/Vs, and we thus observed an ultra-strong Shubnikov-de Haas oscillation in the longitudinal resistivity, as well as the Hall steps in transverse resistivity below 14 T. Our transport and angular resolved photoemission spectroscopy results suggest that the rare-earth and transition metal co-doping in Bi2Se3 system is a promising avenue implement the quantum anomalous Hall effect, as well as harnessing the massive Dirac fermion in electrical devices., Comment: 5 figures

Moire superlattices formed in van der Waals heterostructures due to twisting, lattice mismatch and strain present an opportunity for creating novel metamaterials with unique properties not present in the individual layers themselves. Ferroelectricity for example, arises due to broken inversion symmetry in twisted and strained bilayers of 2D semiconductors with stacking domains of alternating out-of-plane polarization. However, understanding the individual contributions of twist and strain to the formation of topological polar nanostructures remains to be established and has proven to be experimentally challenging. Inversion symmetry breaking has been predicted to give rise to an in-plane component of polarization along the domain walls, leading to the formation of a network of topologically non-trivial merons (half-skyrmions) that are Bloch-type for twisted and Neel-type for strained systems. Here we utilise angle-resolved, high-resolution vector piezoresponse force microscopy (PFM) to spatially resolve polarization components and topological polar nanostructures in marginally twisted bilayer WSe2, and provide experimental proof for the existence of topologically non-trivial meron/antimeron structures. We observe both Bloch-type and Neel-type merons, allowing us to differentiate between moire superlattices formed due to twist or heterogeneous strain. This first demonstration of non-trivial real-space topology in a twisted van der Waals heterostructure opens pathways for exploring the connection between twist and topology in engineered nano-devices.

Nanoscale detection and control of the magnetic order underpins a broad spectrum of fundamental research and practical device applications. The key principle involved is the breaking of time-reversal ($\cal{T}$) symmetry, which in ferromagnets is generated by an internal magnetization. However, the presence of a net-magnetization also imposes severe limitations on compatibility with other prominent phases ranging from superconductors to topological insulators, as well as on spintronic device scalability. Recently, altermagnetism has been proposed as a solution to this restriction, since it shares the enabling $\cal{T}$-symmetry breaking characteristic of ferromagnetism, combined with the antiferromagnetic-like vanishing net-magnetization. To date, altermagnetic ordering has been inferred from spatially averaged probes. Here, we demonstrate nanoscale imaging and control of altermagnetic ordering ranging from nanoscale vortices to domain walls to microscale single-domain states in MnTe. We combine the $\cal{T}$-symmetry breaking sensitivity of X-ray magnetic circular dichroism with magnetic linear dichroism and photoemission electron microscopy, to achieve detailed imaging of the local altermagnetic ordering vector. A rich variety of spin configurations can be imposed using microstructure patterning or thermal cycling in magnetic fields. The demonstrated detection and control of altermagnetism paves the way for future research ranging from ultra-scalable digital and neuromorphic spintronic devices, to the interplay of altermagnetism with non-dissipative superconducting or topological phases., Comment: 17 pages, 3 figures

Nitrogen vacancy centres in diamond can be used for vector magnetometry. In this work we present a portable vector diamond magnetometer. Its vector capability, combined with feedback control and robust structure enables operation on moving platforms. While placed on a trolley, magnetic mapping of a room is demonstrated and the magnetometer is also shown to be operational in a moving van with the measured magnetic field shifts for the x, y, and z axes being tagged with GPS coordinates. These magnetic field measurements are in agreement with measurements taken simultaneously with a fluxgate magnetometer., Comment: 25 pages, 32 figures

We study quasi-freestanding bilayer graphene on silicon carbide intercalated by calcium. The intercalation, and subsequent changes to the system, were investigated by low-energy electron diffraction, angle-resolved photoemission spectroscopy (ARPES) and density-functional theory (DFT). Calcium is found to intercalate only at the graphene-SiC interface, completely displacing the hydrogen terminating SiC. As a consequence, the system becomes highly n-doped. Comparison to DFT calculations shows that the band dispersion, as determined by ARPES, deviates from the band structure expected for Bernal-stacked bilayer graphene. Instead, the electronic structure closely matches AA-stacked bilayer graphene on Ca-terminated SiC, indicating a spontaneous transition from AB- to AA-stacked bilayer graphene following calcium intercalation of the underlying graphene-SiC interface., Comment: 14 pages, 3 figures

Magnetoelastic effects in antiferromagnetic CuMnAs are investigated by applying dynamic strain in the 0.01% range through surface acoustic waves in the GaAs substrate. The magnetic state of the CuMnAs/GaAs is characterized by a multitude of submicron-sized domains which we image by x-ray magnetic linear dichroism combined with photoemission electron microscopy. Within the explored strain range, CuMnAs shows magnetoelastic effects in the form of N\'eel vector waves with micrometer wavelength, which corresponds to an averaged overall spin-axis rotation up to 2.4 deg driven by the time-dependent strain from the surface acoustic wave. Measurements at different temperatures indicate a reduction of the wave amplitude when lowering the temperature. However, no domain wall motion has been detected on the nanosecond timescale

Magnesium intercalated 'quasi-freestanding' bilayer graphene on 6H-SiC(0001) (Mg-QFSBLG) has many favorable properties (e.g., highly n-type doped, relatively stable in ambient conditions). However, intercalation of Mg underneath monolayer graphene is challenging, requiring multiple intercalation steps. Here, we overcome these challenges and subsequently increase the rate of Mg intercalation by laser patterning (ablating) the graphene to form micron-sized discontinuities. We then use low energy electron diffraction to verify Mg-intercalation and conversion to Mg-QFSBLG, and X-ray photoelectron spectroscopy to determine the Mg intercalation rate for patterned and non-patterned samples. By modeling Mg intercalation with the Verhulst equation, we find that the intercalation rate increase for the patterned sample is 4.5$\pm$1.7. Since the edge length of the patterned sample is $\approx$5.2 times that of the non-patterned sample, the model implies that the increased intercalation rate is proportional to the increase in edge length. Moreover, Mg intercalation likely begins at graphene discontinuities in pristine samples (not step edges or flat terraces), where the 2D-like crystal growth of Mg-silicide proceeds. Our laser patterning technique may enable the rapid intercalation of other atomic or molecular species, thereby expanding upon the library of intercalants used to modify the characteristics of graphene, or other 2D materials and heterostructures., Comment: 24 pages, 4 figures

Topological insulators are emerging materials with insulating bulk and symmetry protected nontrivial surface states. One of the most fascinating transport behaviors in a topological insulator is the quantized anomalous Hall insulator, which has been observed inmagnetic-topological-insulator-based devices. In this work, we report a successful doping of rare earth element Tb into Bi$_{1.08}$Sb$_{0.9}$Te$_2$S topological insulator single crystals, in which the Tb moments are antiferromagnetically ordered below ~10 K. Benefiting from the in-bulk-gap Fermi level, transport behavior dominant by the topological surface states is observed below ~ 150 K. At low temperatures, strong Shubnikov-de Haas oscillations are observed, which exhibit 2D-like behavior. The topological insulator with long range magnetic ordering in rare earth doped Bi$_{1.08}$Sb$_{0.9}$Te$_2$S single crystal provides an ideal platform for quantum transport studies and potential applications., Comment: 15 pages, 3 figures

Chalcogen vacancies in transition metal dichalcogenides are widely acknowledged as both donor dopants and as a source of disorder. The electronic structure of sulphur vacancies in MoS2 however is still controversial, with discrepancies in the literature pertaining to the origin of the in-gap features observed via scanning tunneling spectroscopy (STS) on single sulphur vacancies. Here we use a combination of scanning tunnelling microscopy (STM) and STS to study embedded sulphur vacancies in bulk MoS2 crystals. We observe spectroscopic features dispersing in real space and in energy, which we interpret as tip position- and bias-dependent ionization of the sulphur vacancy donor due to tip induced band bending (TIBB). The observations indicate that care must be taken in interpreting defect spectra as reflecting in-gap density of states, and may explain discrepancies in the literature., Comment: 7 pages, 5 figures

Vector magnetometry provides more information than scalar measurements for magnetic surveys utilized in space, defense, medical, geological and industrial applications. These areas would benefit from a mobile vector magnetometer that can operate in extreme conditions. Here we present a scanning fiber-coupled nitrogen vacancy (NV) center vector magnetometer. Feedback control of the microwave excitation frequency is employed to improve dynamic range and maintain sensitivity during movement of the sensor head. Tracking of the excitation frequency shifts for all four orientations of the NV center allow us to image the vector magnetic field of a damaged steel plate. We calculate the magnetic tensor gradiometry images in real time, and they allow us to detect smaller damage than is possible with vector or scalar imaging., Comment: 6 pages, 5 figures

Altermagnetism is a recently identified magnetic symmetry class combining characteristics of conventional collinear ferromagnets and antiferromagnets, that were regarded as mutually exclusive, and enabling phenomena and functionalities unparalleled in either of the two traditional elementary magnetic classes. In this work we use symmetry and ab initio theory to explore X-ray magnetic circular dichroism (XMCD) in the altermagnetic class. Our results highlight the distinct phenomenology in altermagnets of this time-reversal symmetry breaking response, and its potential utility for element-specific spectroscopy and microscopy in altermagnets. As a representative material for our XMCD study we choose $\alpha$-MnTe with the compensated antiparallel magnetic order in which an anomalous Hall effect has been already demonstrated both in theory and experiment. The predicted magnitude of XMCD lies well within the resolution of existing experimental techniques., Comment: Experimental data added

Antiferromagnetic materials hold potential for use in spintronic devices with fast operation frequencies and field robustness. Despite the rapid progress in proof-of-principle functionality in recent years, there has been a notable lack of understanding of antiferromagnetic domain formation and manipulation, which translates to either incomplete or non-scalable control of the magnetic order. Here, we demonstrate simple and functional ways of influencing the domain structure in CuMnAs and Mn2Au, two key materials of antiferromagnetic spintronics research, using device patterning and strain engineering. Comparing x-ray microscopy data from two different materials, we reveal the key parameters dictating domain formation in antiferromagnetic devices and show how the non-trivial interaction of magnetostriction, substrate clamping and edge anisotropy leads to specific equilibrium domain configurations. More specifically, we observe that patterned edges have a significant impact on the magnetic anisotropy and domain structure over long distances, and we propose a theoretical model that relates short-range edge anisotropy and long-range magnetoelastic interactions. The principles invoked are of general applicability to the domain formation and engineering in antiferromagnetic thin films at large, which will pave the way towards realizing truly functional antiferromagnetic devices., Comment: 31 pages, 7 figures

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral one-dimensional edge states. Yet, in magnetic topological insulators (MTI) to date, topological protection is far from robust, with the zero-magnetic field QAH effect only realised at temperatures an order of magnitude below the N\'eel temperature TN, though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realising QAH effect at higher temperatures. Here we use a scanning tunnelling microscope to directly map the size of the exchange gap (Eg,ex) and its spatial fluctuation in the QAH insulator 5-layer MnBi$_2$Te$_4$. We observe long-range fluctuations of Eg,ex with values ranging between 0 (gapless) and 70 meV, uncorrelated to individual point defects. We directly image the breakdown of topological protection, showing that the chiral edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless metallic regions in the bulk. Finally, we unambiguously demonstrate that the gapless regions originate in magnetic disorder, by demonstrating that a small magnetic field restores Eg,ex in these regions, explaining the recovery of topological protection in magnetic fields. Our results indicate that overcoming magnetic disorder is key to exploiting the unique properties of QAH insulators.

The spin readout of an ensemble of nitrogen-vacancy (NV) centers in diamond can be realized by a photoconductive detection that is a complementary method to the optical detection of the NV electron spin magnetic resonance. Here, we implement the photoconductive detection through graphitic planar electrodes that collect the photocurrent. Graphitic electrodes are patterned using a xenon Focused-Ion Beam on an Optical-Grade quality diamond crystal containing a nitrogen concentration of ~1 ppm and a NV concentration of a few ppb. Resistance and current-voltage characteristics of the NV-doped diamond junction are investigated tuning the 532 nm pump beam intensity. The junction has an ohmic behavior and under a strong bias field, we observe velocity saturation of the optically-induced carriers in the diamond junction. We perform the photoconductive detection in continuous-wave regime of the magnetic resonance of the NV centers ensemble for a magnetic field applied along the <100> and the <111> direction with a magnitude above 100 mT. This technique enables the realization of all-carbon diamond quantum sensors integrating graphitic microstructures for the electrical readout., Comment: 11 pages, 3 figures, the following article has been submitted to Applied Physics Letters

Ensembles of nitrogen vacancy centres (NVCs) in diamond can be employed for sensitive magnetometry. In this work we present a fiber-coupled NVC magnetometer with an unshielded sensitivity of (30 $\pm$ 10) pT/$\sqrt{\textrm{Hz}}$ in a (10 - 500)-Hz frequency range. This sensitivity is enabled by a relatively high green-to-red photon conversion efficiency, the use of a [100] bias field alignment, microwave and lock-in amplifier (LIA) parameter optimisation, as well as a balanced hyperfine excitation scheme. Furthermore, a silicon carbide (SiC) heat spreader is used for microwave delivery, alongside low-strain $^{12}\textrm{C}$ diamonds, one of which is placed in a second magnetically insensitive fluorescence collecting sensor head for common-mode noise cancellation. The magnetometer is capable of detecting signals from sources such as a vacuum pump up to 2 m away, with some orientation dependence but no complete dead zones, demonstrating its potential for use in remote sensing applications., Comment: 21 pages, 19 figures, correction to data analysis

Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communication and unfavorable for imaging in biological tissues. Here, we report the experimental observation of a new color center that emits in the telecom O-band, which we observe in silicon-doped bulk single crystal diamonds and microdiamonds. Combining absorption and photoluminescence measurements, we identify a zero-phonon line at 1221 nm and phonon replicas separated by 42 meV. Using transient absorption spectroscopy, we measure an excited state lifetime of around 270 ps and observe a long-lived baseline that may arise from intersystem crossing to another spin manifold.

Strain-induced pseudo magnetic fields offer the possibility of realizing zero magnetic field Quantum Hall effect in graphene, possibly up to room temperature, representing a promising avenue for lossless charge transport applications. Strain engineering on graphene has been achieved via random nanobubbles or artificial nanostructures on the substrate, but the highly localized and non-uniform pseudomagnetic fields can make spectroscopic probes of electronic structure difficult. Heterostructure engineering offers an alternative approach: By stacking graphene on top of another van der Waals material with large lattice mismatch at a desired twist angle, it is possible to generate large strain-induced pseudo magnetic fields uniformly over the entire heterostructure. Here, we report using nano-angle resolved photoemission spectroscopy (nano-ARPES) to probe the electronic bandstructure of a graphene/black phosphorus heterostructure (G/BP). By directly measuring the iso-energy contours of graphene and black phosphorus we determine a twist angle of 20-degrees in our heterostructure. High-resolution nano-ARPES of the graphene bands near the Fermi level reveals the emergence of flat bands located within the Dirac cone. The spacing of the flat bands is consistent with Landau level formation in graphene, and corresponds to a pseudo-field of 11.36 T. Our work provides a new way to study quantum Hall phases induced by strain in 2D materials and heterostructures.

We describe measurements of the uniaxial magnetic anisotropy and spin-flop rotation of the N\'eel vector in antiferromagnetic CuMnAs thin films using neutron diffraction. The suppression of the magnetic (100) peak under magnetic fields is observed for films as thin as 20 nm indicating that they undergo a spin-flop transition. Good agreement is found between neutron diffraction and electron transport measurements of the spin-flop rotation in the same layer, with a similar shape and hysteresis of the obtained curves, while the neutron measurements provide a quantitative determination of the spin flop extent throughout the antiferromagnet layer., Comment: 5 pages, 4 figures, includes supplementary information

Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum network applications because of their exceptional optical properties and spin coherence. However, the stabilization of SiV0 centers requires careful Fermi level engineering of the diamond host material, making further technological development challenging. Here, we show that SiV0 centers can be efficiently stabilized by photoactivated itinerant carriers. Even in this nonequilibrium configuration, the resulting SiV0 centers are stable enough to allow for resonant optical excitation and optically detected magnetic resonance. Our results pave the way for on-demand generation of SiV0 centers as well as other emerging quantum defects in diamond.

Topologically protected magnetic textures, such as skyrmions, half-skyrmions (merons) and their antiparticles, constitute tiny whirls in the magnetic order. They are promising candidates for information carriers in next-generation memory devices, as they can be efficiently propelled at very high velocities using current-induced spin torques. Antiferromagnets have been shown to host versions of these textures, which have gained significant attention because of their potential for terahertz dynamics, deflection free motion, and improved size scaling due to the absence of stray field. Here we show that topological spin textures, merons and antimerons, can be generated at room temperature and reversibly moved using electrical pulses in thin film CuMnAs, a semimetallic antiferromagnet that is a testbed system for spintronic applications. The electrical generation and manipulation of antiferromagnetic merons is a crucial step towards realizing the full potential of antiferromagnetic thin films as active components in high density, high speed magnetic memory devices., Comment: 11 pages, 4 figures

The surface area of Bi2Te3 thin films was increased by introducing nanoscale porosity. Temperature dependent resistivity and magnetotransport measurements were conducted both on as-grown and porous samples (23 and 70 nm). The longitudinal resistivity of the porous samples became more metallic, indicating the increased surface area resulted in transport that was more surface-like. Weak antilocalization (WAL) was present in all samples, and remarkably the phase coherence length doubled in the porous samples. This increase is likely due to the large Fermi velocity of the Dirac surface states. Our results show that the introduction of nanoporosity does not destroy the topological surface states but rather enhances them, making these nanostructured materials promising for low energy electronics, spintronics and thermoelectrics.

Efficient manipulation of antiferromagnetic (AF) domains and domain walls has opened up new avenues of research towards ultrafast, high-density spintronic devices. AF domain structures are known to be sensitive to magnetoelastic effects, but the microscopic interplay of crystalline defects, strain and magnetic ordering remains largely unknown. Here, we reveal, using photoemission electron microscopy combined with scanning X-ray diffraction imaging and micromagnetic simulations, that the AF domain structure in CuMnAs thin films is dominated by nanoscale structural twin defects. We demonstrate that microtwin defects, which develop across the entire thickness of the film and terminate on the surface as characteristic lines, determine the location and orientation of 180 degree and 90 degree domain walls. The results emphasize the crucial role of nanoscale crystalline defects in determining the AF domains and domain walls, and provide a route to optimizing device performance.

Understanding the air-stability of MnBi$_2$Te$_4$ thin films is crucial for the development and long-term operation of electronic devices based around magnetic topological insulators. In the present work, we study MnBi$_2$Te$_4$ thin films upon exposure to atmosphere using a combination of synchrotron-based photoelectron spectroscopy, room temperature electrical transport and atomic force microscopy to determine the oxidation process. After 2 days air exposure a 2 nm thick oxide passivates the surface, corresponding to oxidation of only the top two surface layers, with the underlying layers preserved. This protective oxide layer results in samples that still exhibit metallic conduction even after several days air exposure. Furthermore, the work function decreases from 4.4 eV for pristine MnBi$_2$Te$_4$ to 4.0 eV after the formation of the oxide, along with only a small shift in the core levels indicating minimal doping as a result of air exposure. With the oxide confined to the top surface layers, and the underlying layers preserved, it may be possible to explore new avenues in how to handle, prepare and passivate future MnBi$_2$Te$_4$ devices.

The recently discovered electrical-induced switching of antiferromagnetic (AF) materials that have spatial inversion asymmetry has enriched the field of spintronics immensely and opened the door for the concept of antiferromagnetic MRAM. CuMnAs is one promising AF material that exhibits such electrical switching ability, and has been studied to switch using electrical pulses of length millisecond down to picosecond, but with little focus on nanosecond regime. We demonstrate here switching of CuMnAs/GaP using nanosecond pulses. Our results showed that in the nanosecond regime low-energy switching, high readout signal with highly reproducible behaviour down to a single pulse can be achieved. Moreover, a comparison of the two switching methods of orthogonal switching and polarity switching was done on same device showing two different behaviours that can be exploited selectively for different future memory/processing applications.

Combining magnetism and nontrivial band topology gives rise to quantum anomalous Hall (QAH) insulators and exotic quantum phases such as the QAH effect where current flows without dissipation along quantized edge states. Inducing magnetic order in topological insulators via proximity to a magnetic material offers a promising pathway towards achieving QAH effect at high temperature for lossless transport applications. One promising architecture involves a sandwich structure comprising two single layers of MnBi2Te4 (a 2D ferromagnetic insulator) with ultra-thin Bi2Te3 in the middle, and is predicted to yield a robust QAH insulator phase with a bandgap well above thermal energy at room temperature (25 meV). Here we demonstrate the growth of a 1SL MnBi2Te4 / 4QL Bi2Te3 /1SL MnBi2Te4 heterostructure via molecular beam epitaxy, and probe the electronic structure using angle resolved photoelectron spectroscopy. We observe strong hexagonally warped massive Dirac Fermions and a bandgap of 75 meV. The magnetic origin of the gap is confirmed by the observation of broken time reversal symmetry and the exchange-Rashba effect, in excellent agreement with density functional theory calculations. These findings provide insights into magnetic proximity effects in topological insulators, that will move lossless transport in topological insulators towards higher temperature., Comment: 24 pages

Inducing long-range magnetic order in three-dimensional topological insulators can gap the Diraclike metallic surface states, leading to exotic new phases such as the quantum anomalous Hall effect or the axion insulator state. These magnetic topological phases can host robust, dissipationless charge and spin currents or unique magnetoelectric behavior, which can be exploited in low-energy electronics and spintronics applications. Although several different strategies have been successfully implemented to realize these states, to date these phenomena have been confined to temperatures below a few Kelvin. In this review, we focus on one strategy, inducing magnetic order in topological insulators by proximity of magnetic materials, which has the capability for room temperature operation, unlocking the potential of magnetic topological phases for applications. We discuss the unique advantages of this strategy, the important physical mechanisms facilitating magnetic proximity effect, and the recent progress to achieve, understand, and harness proximity-coupled magnetic order in topological insulators. We also highlight some emerging new phenomena and applications enabled by proximity coupling of magnetism and topological materials, such as skyrmions and the topological Hall effect, and we conclude with an outlook on remaining challenges and opportunities in the field., Comment: Review article, 30 pages including references, 11 figures

The interest in understanding scaling limits of magnetic textures such as domain walls spans the entire field of magnetism from its relativistic quantum fundamentals to applications in information technologies. The traditional focus of the field on ferromagnets has recently started to shift towards antiferromagnets which offer a rich materials landscape and utility in ultra-fast and neuromorphic devices insensitive to magnetic field perturbations. Here we report the observation that domain walls in an epitaxial crystal of antiferromagnetic CuMnAs can be atomically sharp. We reveal this ultimate domain wall scaling limit using differential phase contrast imaging within aberrationcorrected scanning transmission electron microscopy, which we complement by X-ray magnetic dichroism microscopy and ab initio calculations. We highlight that the atomically sharp domain walls are outside the remits of established spin-Hamiltonian theories and can offer device functionalities unparalleled in ferromagnets., Comment: 8 pages, 4 figures, Supplementary information

Intrinsic magnetic topological insulators offer low disorder and large magnetic bandgaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the Quantum Anomalous Hall (QAH) effect and axion insulator phases have been realised. These observations occur at temperatures significantly lower than the Neel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultra-thin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verifying whether the gap is magnetic in the QAH phase. Here we utilise temperature dependent angle-resolved photoemission spectroscopy to study epitaxial ultra-thin MnBi2Te4. We directly observe a layer dependent crossover from a 2D ferromagnetic insulator with a bandgap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>100 meV) at 8 K in 3 and 5 SL MnBi2Te4. The QAH gap is confirmed to be magnetic in origin, as it abruptly diminishes with increasing temperature above 8 K. The direct observation of a large magnetic energy gap in the QAH phase of few-SL MnBi2Te4 is promising for further increasing the operating temperature of QAH materials.

We experimentally measure the band dispersions of topological Dirac semimetal Na3Bi using Fourier-transform scanning tunneling spectroscopy to image quasiparticle interference on the (001) surface of molecular-beam epitaxy-grown Na3Bi thin films. We find that the velocities for the lowest-lying conduction and valencebands are 1.6x10^6 m/s and 4.2x10^5 m/s respectively, significantly higher than previous theoreticalpredictions. We compare the experimental band dispersions to the theoretical band structures calculated usingan increasing hierarchy of approximations of self-energy corrections due to interactions: generalized gradientapproximation (GGA), meta-GGA, Heyd-Scuseria-Ernzerhof exchange-correlation functional (HSE06), and GW methods. We find that density functional theory methods generally underestimate the electron velocities. However, we find significantly improved agreement with an increasingly sophisticated description of the exchange and interaction potential, culminating in reasonable agreement with experiments obtained by the GW method. The results indicate that exchange-correlation effects are important in determining the electronicstructure of this Na3Bi, and are likely the origin of the high velocity. The electron velocity is consistent withrecent experiments on ultrathin Na3Bi and also may explain the ultrahigh carrier mobility observed in heavilyelectron-doped Na3Bi.

Antiferromagnets offer spintronic device characteristics unparalleled in ferromagnets owing to their lack of stray fields, THz spin dynamics, and rich materials landscape. Microscopic imaging of aniferromagnetic domains is one of the key prerequisites for understading physical principles of the device operation. However, adapting common magnetometry techniques to the dipolar-field-free antiferromagnets has been a major challenge. Here we demonstrate in a collinear antiferromagnet a thermoelectric detection method by combining the magneto-Seebeck effect with local heat gradients generated by scanning far-field or near-field techniques. In a 20 nm epilayer of uniaxial CuMnAs we observe reversible 180 deg switching of the N\'eel vector via domain wall displacement, controlled by the polarity of the current pulses. We also image polarity-dependent 90 deg switching of the N\'eel vector in a thicker biaxial film, and domain shattering induced at higher pulse amplitudes. The antiferromagnetic domain maps obtained by our laboratory technique are compared to measurements by the established synchrotron microscopy using X-ray magnetic linear dichroism.

Ensembles of nitrogen-vacancy (NV) centers in diamond are a leading platform for practical quantum sensors. Reproducible and scalable fabrication of NV-ensembles with desired properties is crucial. This work addresses these challenges by developing a chemical vapor deposition (CVD) synthesis process to produce diamond material at scale with improved NV-ensemble properties for a target NV density. The material reported in this work enables immediate sensitivity improvements for current devices. In addition, techniques established in this work for material and sensor characterization at different stages of the CVD synthesis process provide metrics for future efforts targeting other NV densities or sample geometries., Comment: 16 pages, 10 figures, 5 tables

The intercalation of epitaxial graphene on SiC(0001) with Ca has been studied extensively, yet precisely where the Ca resides remains elusive. Furthermore, the intercalation of Mg underneath epitaxial graphene on SiC(0001) has not been reported. Here, we use low energy electron diffraction, x-ray photoelectron spectroscopy, secondary electron cut-off photoemission and scanning tunneling microscopy to elucidate the physical and electronic structure of both Ca- and Mg-intercalated epitaxial graphene on 6H-SiC(0001). We find that Ca intercalates underneath the buffer layer and bonds to the Si-terminated SiC surface, breaking the C-Si bonds of the buffer layer i.e. 'freestanding' the buffer layer to form Ca-intercalated quasi-freestanding bilayer graphene (Ca-QFSBLG). The situation is similar for the Mg-intercalation of epitaxial graphene on SiC(0001), where an ordered Mg-terminated reconstruction at the SiC surface and Mg bonds to the Si-terminated SiC surface are formed, resulting in Mg-intercalated quasi-freestanding bilayer graphene (Mg-QFSBLG). Ca-intercalation underneath the buffer layer has not been considered in previous studies of Ca-intercalated epitaxial graphene. Furthermore, we find no evidence that either Ca or Mg intercalates between graphene layers. However, we do find that both Ca-QFSBLG and Mg-QFSBLG exhibit very low workfunctions of 3.68 and 3.78 eV, respectively, indicating high n-type doping. Upon exposure to ambient conditions, we find Ca-QFSBLG degrades rapidly, whereas Mg-QFSBLG remains remarkably stable., Comment: 58 pages, 10 figures, 4 tables. Revised text and figures

Na3Bi has attracted significant interest in both bulk form as a three-dimensional topological Dirac semimetal and in ultra-thin form as a wide-bandgap two-dimensional topological insulator. Its extreme air sensitivity has limited experimental efforts on thin- and ultra-thin films grown via molecular beam epitaxy to ultra-high vacuum environments. Here we demonstrate air-stable Na3Bi thin films passivated with magnesium difluoride (MgF2) or silicon (Si) capping layers. Electrical measurements show that deposition of MgF2 or Si has minimal impact on the transport properties of Na3Bi whilst in ultra-high vacuum. Importantly, the MgF2-passivated Na3Bi films are air-stable and remain metallic for over 100 hours after exposure to air, as compared to near instantaneous degradation when they are unpassivated. Air stability enables transfer of films to a conventional high-magnetic field cryostat, enabling quantum transport measurements which verify that the Dirac semimetal character of Na3Bi films is retained after air exposure.

Recent research works have shown that the magnetic order in some antiferromagnetic materials can be manipulated and detected electrically, due to two physical mechanisms: Neel-order spin-orbit torques and anisotropic magnetoresistance. While these observations open up opportunities to use antiferromagnets for magnetic memory devices, different physical characterization methods are required for a better understanding of those mechanisms. Here we report a magnetic field induced rotation of the antiferromagnetic Neel vector in epitaxial tetragonal CuMnAs thin films. Using soft x-ray magnetic linear dichroism spectroscopy, x-ray photoemission electron microscopy, integral magnetometry and magneto-transport methods, we demonstrate spin-flop switching and continuous spin reorientation in antiferromagnetic films with uniaxial and biaxial magnetic anisotropies, respectively. From field-dependent measurements of the magnetization and magnetoresistance, we obtain key material parameters including the anisotropic magnetoresistance coefficients, magnetocrystalline anisotropy, spin-flop and exchange fields., Comment: 26 pages, 6 figures

We present a detailed study of the growth of the tetragonal polymorph of antiferromagnetic CuMnAs by the molecular beam epitaxy technique. We explore the parameter space of growth conditions and their effect on the microstructural and transport properties of the material. We identify its typical structural defects and compare the properties of epitaxial CuMnAs layers grown on GaP, GaAs and Si substrates. Finally, we investigate the correlation between the crystalline quality of CuMnAs and its performance in terms of electrically induced resistance switching., Comment: 10 pages, 8 figures and supplementary material

Layered indium selenides ($In_{2}Se_{3}$) have recently been discovered to host robust out-of-plane and in-plane ferroelectricity in the $\alpha$ and $\beta$' phases, respectively. In this work, we utilise angle-resolved photoelectron spectroscopy to directly measure the electronic bandstructure of $\beta '-In_{2}Se_{3}$, and compare to hybrid density functional theory (DFT) calculations. In agreement with DFT, we find the band structure is highly two-dimensional, with negligible dispersion along the c-axis. Due to n-type doping we are able to observe the conduction band minima, and directly measure the minimum indirect (0.97 eV) and direct (1.46 eV) bandgaps. We find the Fermi surface in the conduction band is characterized by anisotropic electron pockets with sharp in-plane dispersion about the $\overline{M}$ points, yielding effective masses of 0.21 $m_{0}$ along $\overline{KM}$ and 0.33 $m_{0}$ along $\overline{\Gamma M}$. The measured band structure is well supported by hybrid density functional theory calculations. The highly two-dimensional (2D) bandstructure with moderate bandgap and small effective mass suggest that $\beta'-In_{2}Se_{3}$ is a potentially useful new van der Waals semiconductor. This together with its ferroelectricity makes it a viable material for high-mobility ferroelectric-photovoltaic devices, with applications in non-volatile memory switching and renewable energy technologies., Comment: 19 pages, 4 + 1 figures; typos corrected;added references; updated figures & discussion to reflect changes in model

Antiferromagnets (AFs) attract much attention due to potential applications in spintronics. Both the electric current and the electric field are considered as tools suitable to control properties and the N\'eel vector direction of AFs. Among AFs, CuMnAs has been shown to exhibit specific properties that result in the existence of the current-induced spin-orbit torques commensurate with spin directions and topological Dirac quasiparticles. Here, we report on the observation of a reversible effect of an electric field on the resistivity of CuMnAs thin films, employing ionic liquid as a gate insulator. The data allow to determine the carrier type, concentration, and mobility independently of the Hall effect that may be affected by an anomalous component.

A two-dimensional topological insulator (2DTI) has an insulating bulk and helical spin-polarised edge modes robust to backscattering by non-magnetic disorder. While ballistic transport has been demonstrated in 2DTIs over short distances, larger samples show significant backscattering and a nearly temperature-independent resistance whose origin is unclear. 2DTI edges have shown a spin polarisation, however the degree of helicity is difficult to quantify from spin measurements. Here, we study 2DTI few-layer Na3Bi on insulating Al2O3. A non-local conductance measurement geometry enables sensitive detection of the edge conductance in the topological regime, with an edge mean free path ~100 nm. Magnetic field suppresses spin-flip scattering in the helical edges, resulting in a giant negative magnetoresistance (GNMR), up to 80% at 0.9 T. Comparison to theory indicates >98% of scattering is helical spin scattering significantly exceeding the maximum (67%) expected for a non-helical metal. GNMR, coupled with non-local measurements demonstrating edge conduction, thus provides an unambiguous experimental signature of helical edges that we expect to be generically useful in understanding 2DTIs.

The electric field induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor [1-4]. In this scheme an electric field can switch 'on' the ballistic flow of charge and spin along dissipationless edges of the two-dimensional (2D) quantum spin Hall insulator [5-9], and when 'off' is a conventional insulator with no conductive channels. Such as topological transistor is promising for low-energy logic circuits [4], which would necessitate electric field-switched materials with conventional and topological bandgaps much greater than room temperature, significantly greater than proposed to date [6-8]. Topological Dirac semimetals(TDS) are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases [3,10-16]. Here we use scanning probe microscopy/spectroscopy (STM/STS) and angle-resolved photoelectron spectroscopy (ARPES) to show that mono- and bilayer films of TDS Na3Bi [3,17] are 2D topological insulators with bulk bandgaps >400 meV in the absence of electric field. Upon application of electric field by doping with potassium or by close approach of the STM tip, the bandgap can be completely closed then re-opened with conventional gap greater than 100 meV. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy kT = 25 meV at room temperature, suggest that ultrathin Na3Bi is suitable for room temperature topological transistor operation.

Electrical current-induced deterministic magnetization switching in a magnetic multilayer structure without external magnetic field is realized by utilizing interlayer exchange coupling. Two ferromagnetic Co layers, with in-plane and out-of-plane anisotropy respectively, are separated by a spacer Ta layer, which plays a dual role of inducing antiferromagnetic interlayer coupling, and contributing to the current-induced effective magnetic field through the spin Hall effect. The current-induced magnetization switching behavior can be tuned by pre-magnetizing the in-plane Co layer. The antiferromagnetic exchange coupling field increases with decreasing thickness of the Ta layer, reaching 630+-5 Oe for a Ta thickness of 1.5nm. The magnitude of the current-induced perpendicular effective magnetic field from spin-orbit torque is 9.2 Oe/(107Acm-2). The large spin Hall angle of Ta, opposite in sign to that of Pt, results in a low critical current density of 9*10^6A/cm^2. This approach is promising for the electrical switching of magnetic memory elements without external magnetic field.

Antiferromagnets have a number of favourable properties as active elements in spintronic devices, including ultra-fast dynamics, zero stray fields and insensitivity to external magnetic fields . Tetragonal CuMnAs is a testbed system in which the antiferromagnetic order parameter can be switched reversibly at ambient conditions using electrical currents . In previous experiments, orthogonal in-plane current pulses were used to induce 90 degree rotations of antiferromagnetic domains and demonstrate the operation of all-electrical memory bits in a multi-terminal geometry . Here, we demonstrate that antiferromagnetic domain walls can be manipulated to realize stable and reproducible domain changes using only two electrical contacts. This is achieved by using the polarity of the current to switch the sign of the current-induced effective field acting on the antiferromagnetic sublattices. The resulting reversible domain and domain wall reconfigurations are imaged using x-ray magnetic linear dichroism microscopy, and can also be detected electrically. The switching by domain wall motion can occur at much lower current densities than those needed for coherent domain switching., Comment: 8 pages, 4 figures

Color centers in diamond are a promising platform for quantum technologies, and understanding their interactions with the environment is crucial for these applications. We report a study of spin- lattice relaxation (T1) of the neutral charge state of the silicon vacancy center in diamond. Above 20 K, T1 decreases rapidly with a temperature dependence characteristic of an Orbach process, and is strongly anisotropic with respect to magnetic field orientation. As the angle of the magnetic field is rotated relative to the symmetry axis of the defect, T1 is reduced by over three orders of magnitude. The electron spin coherence time (T2) follows the same temperature dependence but is drastically shorter than T1. We propose that these observations result from phonon-mediated transitions to a low lying excited state that are spin conserving when the magnetic field is aligned with the defect axis, and we discuss likely candidates for this excited state.

We study the temperature dependence ($77$ K - $475$ K) of the longitudinal resistivity and Hall coefficient of thin films (thickness $20$ nm) of three dimensional topological Dirac semimetal Na$_3$Bi grown via molecular beam epitaxy (MBE). The temperature-dependent Hall coefficient is electron-like at low temperature, but transitions to hole-like transport around $200$ K. We develop a model of a Dirac band with electron-hole asymmetry in Fermi velocity and mobility (assumed proportional to the square of Fermi velocity) which explains well the magnitude and temperature dependence of the Hall resistivity. We find that the hole mobility is about $7$ times larger than the electron mobility. In addition, we find that the electron mobility decreases significantly with increasing temperature, suggesting electron-phonon scattering strongly limits the room temperature mobility., Comment: 12 pages

The silicon-vacancy center in diamond offers attractive opportunities in quantum photonics due to its favorable optical properties and optically addressable electronic spin. Here, we combine both to achieve all-optical coherent control of its spin states. We utilize this method to explore spin dephasing effects in an impurity-rich sample beyond the limit of phonon-induced decoherence: Employing Ramsey and Hahn-echo techniques at 12mK base temperature we identify resonant coupling to a substitutional nitrogen spin bath as the limiting decoherence source for the electron spin.

Large-area thin films of topological Dirac semimetal Na$_3$Bi are grown on amorphous SiO$_2$:Si substrates to realise a field-effect transistor with the doped Si acting as back gate. As-grown films show charge carrier mobilities exceeding 7,000 cm$^2$/Vs and carrier densities below 3 $\times $10$^{18}$ cm$^{-3}$, comparable to the best thin-film Na$_3$Bi. An ambipolar field effect and minimum conductivity are observed, characteristic of Dirac electronic systems. The results are quantitatively understood within a model of disorder-induced charge inhomogeneity in topological Dirac semimetals. Due to the inverted band structure, the hole mobility is significantly larger than the electron mobility in Na$_3$Bi, and when present, these holes dominate the transport properties., Comment: 5 pages, 4 figures; minor corrections and revisions for readability

3D Dirac semimetals are an emerging class of materials that possess topological electronic states with a Dirac dispersion in their bulk. In nodal-line Dirac semimetals, the conductance and valence bands connect along a closed path in momentum space, leading to the prediction of pseudospin vortex rings and pseudospin skyrmions. Here, we use Fourier transform scanning tunneling spectroscopy (FT-STS) at 4.5 K to resolve quasiparticle interference (QPI) patterns at single defect centers on the surface of the line nodal semimetal zirconium silicon sulfide (ZrSiS). Our QPI measurements show pseudospin conservation at energies close to the line node. In addition, we determine the Fermi velocity to be $\hbar v_F = 2.65 \pm 0.10$ eV {\AA} in the {\Gamma}-M direction ~300 meV above the Fermi energy $E_F$, and the line node to be ~140 meV above $E_F$. More importantly, we find that certain scatterers can introduce energy-dependent non-preservation of pseudospins, giving rise to effective scattering between states with opposite valley pseudospin deep inside valence and conduction bands. Further investigations of quasiparticle interference at the atomic level will aid defect engineering at the synthesis level, needed for the development of lower-power electronics via dissipationless electronic transport in the future.

Engineering coherent systems is a central goal of quantum science. Color centers in diamond are a promising approach, with the potential to combine the coherence of atoms with the scalability of a solid state platform. However, the solid environment can adversely impact coherence. For example, phonon- mediated spin relaxation can induce spin decoherence, and electric field noise can change the optical transition frequency over time. We report a novel color center with insensitivity to both of these sources of environmental decoherence: the neutral charge state of silicon vacancy (SiV0). Through careful material engineering, we achieve over 80% conversion of implanted silicon to SiV0. SiV0 exhibits excellent spin properties, with spin-lattice relaxation times (T1) approaching one minute and coherence times (T2) approaching one second, as well as excellent optical properties, with approximately 90% of its emission into the zero-phonon line and near-transform limited optical linewidths. These combined properties make SiV0 a promising defect for quantum networks.

We demonstrate optical spin polarization of the neutrally-charged silicon-vacancy defect in diamond ($\mathrm{SiV^{0}}$), an $S=1$ defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but non-zero at below-resonant energies. We measure an ensemble spin coherence time $T_2>100~\mathrm{\mu s}$ at low-temperature, and a spin relaxation limit of $T_1>25~\mathrm{s}$. Optical spin state initialization around 946 nm allows independent initialization of $\mathrm{SiV^{0}}$ and $\mathrm{NV^{-}}$ within the same optically-addressed volume, and $\mathrm{SiV^{0}}$ emits within the telecoms downconversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that $\mathrm{SiV^{0}}$ is a promising candidate for a long-range quantum communication technology.