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Recent observation of anomalous Hall effect (AHE) induced by magnetic field or spin magnetization lying in the Hall deflection plane has sparked interest in diverse mechanisms for inducing the Hall vector component perpendicular to the applied magnetic field. Such off-diagonal coupling, which is strictly constrained by symmetry of the system, provides new degrees of freedom for engineering Hall responses. However, spontaneous response as extensively studied for out-of-plane AHE remains unexplored. Here we elucidate in-plane AHE in a typical ferromagnetic oxide SrRuO$_3$. The (111)-orientated ultrathin films with in-plane easy axes of spin magnetization exhibit spontaneous AHE at zero field, which is intrinsically coupled to the in-plane spin magnetization and controllable via its direction. Systematic measurements by varying azimuthal and polar field angles further reveal complex Hall responses shaped by higher-order terms allowed by trigonal distortion of the films. Our findings highlight versatile and controllable in-plane Hall responses with out-of-plane orbital ferromagnetism., Comment: 16 pages, 4 figures

Rare earth intermetallic compounds crystallized in AlB$_2$-type and its low-symmetry derivative CeCu$_2$-type structures potentially host diverse frustrated magnetic structures and rich magnetotransport phenomena. We report the film growth of CeCu$_2$-type EuZn$_2$ by molecular beam epitaxy and the observation of topological Hall responses highly contrastive to isostructural EuCd$_2$. While their magnetization curves are rather similar, the topological Hall effect observed in EuZn$_2$ is simpler, with the only one component enhanced at the magnetic transition field. EuZn$_2$ may be a unique system for studying the magnetic domain boundary effect on topological Hall responses among the CeCu$_2$-type rare-earth intermetallic compounds., Comment: 12 pages, 4 figures

SrRuO$_3$ is a prototypical transition metal oxide which hosts rich physical properties including itinerant ferromagnetism, high conductivity, and intrinsic Hall effect originating in the Weyl points. Recently, high-quality SrRuO$_3$ films with residual resistivity ratios of more than 50 have been reported to exhibit quantum oscillations at low temperatures in spite of its strong electron correlation. While the origin of the oscillations has been discussed in relation to Weyl orbits based on the Weyl semimetal band structure, so far experimentally reported results are neither consistent with each other nor with theoretically expected behavior, leaving the origin of the oscillations in SrRuO$_3$ films still elusive. In this report, we have carefully evaluated the quantum oscillations observed in three-dimensional thick SrRuO$_3$ films with a high residual resistivity ratio of RRR = 82. We reveal the coexistence of two oscillation components both derived from two-dimensional electronic states and with slightly different masses, suggesting the involvement of the surface Fermi arc states formed between different Weyl point pairs., Comment: 13 pages, 3 figures

For over a century, the Hall effect, a transverse effect under out-of-plane magnetic field or magnetization, has been a cornerstone for magnetotransport studies and applications. Modern theoretical formulation based on the Berry curvature has revealed the potential that even in-plane magnetic field can induce anomalous Hall effect, but its experimental demonstration has remained difficult due to its potentially small magnitude and strict symmetry requirements. Here we report observation of the in-plane anomalous Hall effect by measuring low-carrier density films of magnetic Weyl semimetal EuCd$_2$Sb$_2$. Anomalous Hall resistance exhibits distinct three-fold rotational symmetry for changes in the in-plane field component, and this can be understood in terms of out-of-plane Weyl points splitting or orbital magnetization induced by in-plane field, as also confirmed by model calculation. Our findings demonstrate the importance of in-plane field to control the Hall effect, accelerating materials development and further exploration of various in-plane field induced phenomena., Comment: 14 pages, 4 figures

We investigate the magnetic order in single crystalline EuCd$_2$Sb$_2$ thin films using a combined theoretical and experimental approach. Resonant elastic x-ray scattering experiments reveal a sharp magnetic peak at $q = (0, 0, \frac{1}{2})$ below $T_N = 7.2$ K, indicative of interlayer antiferromagnetic ordering. Additionally, we observe a weak diffuse magnetic signal centered at $q = (0, 0, 1)$ that persists above $T_N$, up to $T_C \sim 11$ K. Our Monte-Carlo simulations of a classical spin model approximation of the Eu magnetic sublattice demonstrate that the diffuse signal can arise from ferromagnetic coupling in the top few layers due to surface oxidation. On the other hand, the bulk of the sample exhibits antiferromagnetic coupling between layers. Finally, our fit of the model parameters to the magnetic ordering temperatures, shed light on the exchange couplings that are key in stabilizing the observed composite magnetic order., Comment: 7 pages, 4 figures

Technical advancement of oxide molecular beam epitaxy (MBE) has opened new avenues for studying various quantum transport phenomena in correlated transition-metal oxides, as exemplified by the exotic superconductivity of Sr$_2$RuO$_4$ and quantum oscillations of SrRuO$_3$. On the other hand, film research of another Ruddlesden-Popper strontium ruthenate Sr$_3$Ru$_2$O$_7$ which exhibits a unique quantum phase related to metamagnetism in bulk systems did not progress well. Here we report the fabrication of high-quality Sr$_3$Ru$_2$O$_7$ thin films by oxide MBE and the observation of a strain-induced ferromagnetic ground state. The change in magnetic exchange coupling evaluated by first-principles calculations indicates a systematic relation between the compression of the $c$-axis length and induced ferromagnetism. Giant epitaxial strain in high-quality films will be a key to a comprehensive understanding of the magnetism in Ruddlesden-Popper strontium ruthenates Sr$_{n+1}$Ru$_n$O$_{3n+1}$, which sensitively depends on the ratio of in-plane to out-of-plane Ru-Ru distances., Comment: 15 pages, 4 figures

Here we study nonmonotonic features which appear both in magnetoresistivity and anomalous Hall resistivity during the simple magnetization process, by systematically measuring type-II magnetic Weyl semimetal EuCd$_2$Sb$_2$ films over a wide carrier density range. We find that a positive magnetoresistivity hump can be explained as manifestation of a field-linear term in the generalized magnetoconductivity formula including the Berry curvature. As also confirmed by model calculation, the term can be negative and pronounced near the Weyl point energy in the case that the Weyl cones are heavily tilted. Our findings demonstrate extensive effects of the Berry curvature on various magnetotransport in magnetic Weyl semimetals beyond the anomalous Hall effect., Comment: 17 pages, 4 figures

Searching for an ideal magnetic Weyl semimetal hosting only a single pair of Weyl points has been a focal point for systematic clarification of its unique magnetotransport derived from the interplay between topology and magnetization. Among the candidates, triangular-lattice antiferromagnet EuCd$_2$As$_2$ has been attracting special attention due to the prediction of the ideal Weyl semimetal phase in the ferromagnetic state, however, transport properties of low-carrier density samples have remained elusive. Here we report molecular beam epitaxy growth of EuCd$_2$As$_2$ films, achieving low-hole density in the range of $10^{15}$-$10^{16}$ cm$^{-3}$ at low temperature. Transport measurements of such low-carrier density films reveal an insulating behavior with an activation gap of about 200 meV, which persists even in the field-induced ferromagnetic state. Our work provides an important experimental clue that EuCd$_2$As$_2$ is intrinsically insulating, contrary to the previous prediction., Comment: 12 pages, 3 figures

We investigate edge and bulk states in Weyl-orbit based quantum Hall effect by measuring a Corbino-type device fabricated from a topological Dirac semimetal (Cd1-xZnx)3As2 film. Clear quantum Hall plateaus are observed when measuring one-sided terminals of the Corbino-type device. This indicates that edge states of the Weyl-orbit quantum Hall effect form closed trajectories consisting of Fermi arcs and chiral zero modes independently on inner and outer sides. On the other hand, the bulk resistance does not diverge at fields where the quantum Hall plateau appears, suggesting that the Weyl orbits in the bulk region are not completely localized when applying electric current through the bulk region.

The binary ruthenate, RuO$_2$, has been the subject of intense interest due to its itinerant antiferromagnetism and strain-induced superconductivity. The strain mechanism and its effect on the microscopic electronic states leading to the normal and superconducting state, however, remain undisclosed. Here, we investigate highly-strained epitaxial (110) RuO$_2$ films using polarization-dependent oxygen K-edge X-ray absorption spectroscopy (XAS). Through the detection of pre-edge peaks, arising from O:$2p$ - Ru:$4d$ hybridization, we uncover the effects of epitaxial strain on the orbital/electronic structure near the Fermi level. Our data show robust strain-induced shifts of orbital levels and a reduction of hybridization strength. Furthermore, we reveal a pronounced in-plane anisotropy of the electronic structure along the $[110]/[1\bar{1}0]$ directions naturally stemming from the symmetry-breaking epitaxial strain of the substrate. The $B_{2g}$ symmetry component of the epitaxially-enforced strain breaks a sublattice degeneracy, resulting in an increase of the density of states at the Fermi level ($E_F$), possibly paving the way to superconductivity. These results underscore the importance of the effective reduction from tetragonal to orthorhombic lattice symmetry in (110) RuO$_2$ films and its relevance towards the superconducting and magnetic properties.

Large intrinsic anomalous Hall effect (AHE) originating in the Berry curvature has attracted growing attention for potential applications. Recently proposed magnetic Weyl semimetal EuCd$_2$Sb$_{\mathrm{2}}$ provides an excellent platform for controlling the intrinsic AHE because it only hosts a Weyl-points related band structure near the Fermi energy. Here we report the fabrication of EuCd$_2$Sb$_{\mathrm{2}}$ single-crystalline films and control of their anomalous Hall effect by film technique. As also analyzed by first-principles calculations of energy-dependent intrinsic anomalous Hall conductivity, the obtained anomalous Hall effect shows a sharp peak as a function of carrier density, demonstrating clear energy dependence of the intrinsic AHE., Comment: 13 pages, 4 figures

We report fabrication of EuSb$_2$ single-crystalline films and investigation of their quantum transport. First-principles calculations demonstrate that EuSb$_2$ is a magnetic topological nodal-line semimetal protected by nonsymmorphic symmetry. Observed Shubnikov-de Haas oscillations with multiple frequency components exhibit small effective masses and two-dimensional field-angle dependence even in a 250 nm thick film, further suggesting possible contributions of surface states. This finding of the high-mobility magnetic topological semimetal will trigger further investigation of exotic quantum transport phenomena by controlling magnetic order in topological semimetal films., Comment: 14 pages, 4 figures + supplementary 6 pages, 5 figures

We present a study on magnetotransport in films of the topological Dirac semimetal Cd$_{3}$As$_{2}$ doped with Sb grown by molecular beam epitaxy. In our weak antilocalization analysis, we find a significant enhancement of the spin-orbit scattering rate, indicating that Sb doping leads to a strong increase of the pristine band-inversion energy. We discuss possible origins of this large enhancement by comparing Sb-doped Cd$_{3}$As$_{2}$ with other compound semiconductors. Sb-doped Cd$_{3}$As$_{2}$ will be a suitable system for further investigations and functionalization of topological Dirac semimetals., Comment: 16 pages, 4 figures

We report strain engineering of superconductivity in RuO$_2$ singlecrystalline films, which are epitaxially grown on rutile TiO$_2$ and MgF$_2$ substrates with various crystal orientations. Systematic mappings between the superconducting transition temperature and the lattice parameters reveal that shortening of specific ruthenium-oxygen bonds is a common feature among the superconducting RuO$_2$ films. Ab initio calculations of electronic and phononic structures for the strained RuO$_2$ films suggest the importance of soft phonon modes for emergence of the superconductivity. The findings indicate that simple transition metal oxides such as with the rutile structure may be suitable for further exploring superconductivity by controlling phonon modes through the epitaxial strain., Comment: 13 pages, 4 figures + supplementary 3 pages, 3 figures

We have studied fundamental properties of weak-link Sr2RuO4/Sr2RuO4 Josephson junctions fabricated by making a narrow constriction on superconducting Sr2RuO4 films through laser micro-patterning. The junctions show a typical overdamped behavior with much higher critical current density, compared with those previously reported for bulk Sr2RuO4/s-wave superconductor junctions. Observed magnetic field and temperature dependences of the Josephson critical current suggest that the chiral p-wave is unlikely for the superconducting symmetry, encouraging further theoretical calculations of the Sr2RuO4/Sr2RuO4 type junctions., Comment: 14 pages, 4 figures

We report an above-room-temperature ferromagnetic state realized in a proximitized Dirac semimetal, which is fabricated by growing typical Dirac semimetal Cd$_3$As$_2$ films on a ferromagnetic garnet with strong perpendicular magnetization. Observed anomalous Hall conductivity with substantially large Hall angles is found to be almost proportional to magnetization and opposite in sign to it. Theoretical calculations based on first-principles electronic structure also demonstrate that the Fermi-level dependent anomalous Hall conductivity reflects the Berry curvature originating in the split Weyl nodes. The present Dirac-semimetal/ferromagnetic-insulator heterostructure will provide a novel platform for exploring Weyl-node transport phenomena and spintronic functions lately proposed for topological semimetals., Comment: 15 pages, 4 figures

Unconventional surface states protected by non-trivial bulk orders are sources of various exotic quantum transport in topological materials. One prominent example is the unique magnetic orbit, so-called Weyl orbit, in topological semimetals where two spatially separated surface Fermi-arcs are interconnected across the bulk. The recent observation of quantum Hall states in Dirac semimetal Cd3As2 bulks have drawn attention to the novel quantization phenomena possibly evolving from the Weyl orbit. Here we report surface quantum oscillation and its evolution into quantum Hall states in Cd3As2 thin film samples, where bulk dimensionality, Fermi energy, and band topology are systematically controlled. We reveal essential involvement of bulk states in the quantized surface transport and the resultant quantum Hall degeneracy depending on the bulk occupation. Our demonstration of surface transport controlled in film samples also paves a way for engineering Fermi-arc-mediated transport in topological semimetals., Comment: 18 pages, 4 figures

The high-temperature superconductivity in copper oxides emerges under strong influence of spin correlations in doped Mott insulators. Recent discoveries of charge-order (CO) correlations in Y-based hole-doped cuprates as well as in electron-doped cuprates suggest that charge correlations should also play an important role on the electronic states of cuprates, although those correlations have been so far detected mainly by x-ray scattering measurements. Here we show signatures of CO correlations in transport properties of electron-doped cuprates as anomalous enhancement of the metal-to-insulator crossover temperature (Tmin) appears in the limited doping range near the onset of superconductivity, while it decreases exactly when superconductivity sets in. We explain this non-monotonous peak-like behavior of Tmin in terms of the evolution of the electronic states through development of CO correlations and appearance of the hole pockets in the folded Fermi surface, which impact on transport properties consecutively at different locations in the momentum space., Comment: 23 pages, 6 figures, accepted for publication in Physical Review B

The recent discovery of topological Dirac semimetals (DSM) has provoked intense curiosity not only on Weyl physics in solids, but also on topological phase transitions originating from DSM. One example is controlling the dimensionality to realize two-dimensional quantum phases such as quantum Hall and quantum spin Hall states. For investigating these phases, the Fermi level is a key controlling parameter. From this perspective, we report here the carrier-density control of quantum Hall states realized in thin films of DSM Cd3As2. Chemical doping of Zn combined with electrostatic gating has enabled us to tune the carrier density over a wide range and continuously even across the charge neutrality point. Comprehensive analyses of the gate-tuned quantum transport have revealed Landau level formation from linearly dispersed sub-bands and its contribution to the quantum Hall states. Our achievements pave the way also for investigating the low energy physics near the Dirac points of DSM., Comment: 20 pages, 4 figures

Cd3As2 has long been known as a high-mobility semiconductor. The recent finding of a topological semimetal state in this compound has demanded growth of epitaxial films with high crystallinity and controlled thickness. Here we report the structural characterisation of Cd3As2 films grown on SrTiO3 substrates by solid-phase epitaxy at high temperatures up to 600 C by employing optimised capping layers and substrates. The As triangular lattice is epitaxially stacked on the Ti square lattice of the (001) SrTiO3 substrate, producing (112)-oriented Cd3As2 films exhibiting high crystallinity with a rocking-curve width of 0.02 and a high electron mobility exceeding 30,000 cm2/Vs. The systematic characterisation of films annealed at various temperatures allowed us to identify two-step crystallisation processes in which out-of-plane and subsequently in-plane directions occur with increasing annealing temperature. Our findings on the high-temperature crystallisation process of Cd3As2 enable a unique approach for fabricating high-quality Cd3As2 films and elucidating quantum transport by back gating through the SrTiO3 substrate., Comment: 10 pages, 4 figures

As symbolized by the Nobel Prize in Physics 2016, "topology" has been recognized as an essential standpoint to understand and control the physics of condensed matter. This concept may be spreading even into application areas such as novel electronics. In this trend, there has been reported a number of study for the oxide films and heterostructures with topologically non-trivial electronic or magnetic states. In this review, we overview the trends of new topological properties and functionalities in oxide materials with sorting out a number of examples. The technological advances in oxide film growth achieved over the last few decades are now opening the door for harnessing novel topological properties., Comment: 15 pages, 7 figures

One of the key technologies in spintronics is to tame spin-orbit coupling (SOC) that links spin and motion of electrons, giving rise to intriguing magneto-transport properties in itinerant magnets. Prominent examples of such SOC-based phenomena are anomalous and topological Hall effects. However, controlling them by electric field has remained unachieved since electric field tends to be screened in itinerant magnets. Here we demonstrate that both anomalous and topological Hall effects can be modulated by electric field in oxide heterostructures consisting of ferromagnetic SrRuO$_{3}$ and nonmagnetic SrIrO$_{3}$. We observed clear electric-field effect only when SrIrO$_{3}$ is inserted between SrRuO$_{3}$ and a gate dielectric. Our results establish that strong SOC of nonmagnetic materials such as SrIrO$_{3}$ is essential in electrical tuning of these Hall effects and possibly other SOC-related phenomena., Comment: 23 pages, 4 figures; revised version has been published in Nat. Commun. 9, 213 (2018)

A well known semiconductor Cd3As2 has reentered the spotlight due to its unique electronic structure and quantum transport phenomena as a topological Dirac semimetal. For elucidating and controlling its topological quantum state, high-quality Cd3As2 thin films have been highly desired. Here we report the development of an elaborate growth technique of high-crystallinity and high-mobility Cd3As2 films with controlled thicknesses and the observation of quantum Hall effect dependent on the film thickness. With decreasing the film thickness to 10 nm, the quantum Hall states exhibit variations such as a change in the spin degeneracy reflecting the Dirac dispersion with a large Fermi velocity. Details of the electronic structure including subband splitting and gap opening are identified from the quantum transport depending on the confinement thickness, suggesting the presence of a two-dimensional topological insulating phase. The demonstration of quantum Hall states in our high-quality Cd3As2 films paves a road to study quantum transport and device application in topological Dirac semimetal and its derivative phases., Comment: 24 pages, 4 figures + supplementary 13 pages, 13 figures

Epitaxial La doped BaSnO3 films were grown in an adsorption controlled regime by molecular beam epitaxy, where the excess volatile SnOx desorbs from the film surface. A film grown on a (001) DyScO3 substrate exhibited a mobility of 183 cm^2 V^-1 s^-1 at room temperature and 400 cm^2 V^-1 s^-1 at 10 K, despite the high concentration (1.2x10^11 cm^-2) of threading dislocations present. In comparison to other reports, we observe a much lower concentration of (BaO)2 Ruddlesden Popper crystallographic shear faults. This suggests that in addition to threading dislocations that other defects possibly (BaO)2 crystallographic shear defects or point defects significantly reduce the electron mobility.

We describe a tunable low-energy photon source consisting of a laser-driven xenon plasma lamp coupled to a Czerny-Turner monochromator. The combined tunability, brightness, and narrow spectral bandwidth make this light source useful in laboratory-based high-resolution photoemission spectroscopy experiments. The source supplies photons with energies up to ~7 eV, delivering under typical conditions >10^12 ph/s within a 10 meV spectral bandwidth, which is comparable to helium plasma lamps and many synchrotron beamlines. We first describe the lamp and monochromator system and then characterize its output, with attention to those parameters which are of interest for photoemission experiments. Finally, we present angle-resolved photoemission spectroscopy data using the light source and compare its performance to a conventional helium plasma lamp.

An interface between an oxide and an electrolyte gives rise to various processes as exemplified by electrostatic charge accumulation/depletion and electrochemical reactions such as intercalation/decalation under electric field. Here we directly compare typical device operations of those in electric double layer transistor geometry by adopting ${A}$-site vacant perovskite WO$_3$ epitaxial thin films as a channel material and two different electrolytes as gating agent. $\textit{In situ}$ measurements of x-ray diffraction and channel resistance performed during the gating revealed that in both the cases WO$_3$ thin film reaches a new metallic state through multiple phase transitions, accompanied by the change in out-of-plane lattice constant. Electrons are electrostatically accumulated from the interface side with an ionic liquid, while alkaline metal ions are more uniformly intercalated into the film with a polymer electrolyte. We systematically demonstrate this difference in the electrostatic and electrochemical processes, by comparing doped carrier density, lattice deformation behavior, and time constant of the phase transitions., Comment: 25 pages, 6 figures, ACS Applied Matter. in press