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Neuromorphic functionalities in memristive devices are commonly associated with the ability to electrically create local conductive pathways by resistive switching. The archetypal correlated material, VO2, has been intensively studied for its complex electronic and structural phase transition as well as its filament formation under applied voltages. Local structural studies of the filament behavior are often limited due to time-consuming rastering which makes impractical many experiments aimed at investigating large spatial areas or temporal dynamics associated with the electrical triggering of the phase transition. Utilizing Dark Field X-ray Microscopy (DFXM), a novel full-field x-ray imaging technique, we study this complex filament formation process in-operando in VO2 devices from a structural perspective. We show that prior to filament formation, there is a significant gain of the metallic rutile phase beneath the metal electrodes that define the device. We observed that the filament formation follows a preferential path determined by the nucleation sites within the device. These nucleation sites are predisposed to the phase transition and can persistently maintain the high-temperature rutile phase even after returning to room temperature, which can enable a novel training/learning mechanism. Filament formation also appears to follow a preferential path determined by a nucleation site within the device which is predisposed to the rutile transition even after returning to room temperature. Finally, we found that small isolated low-temperature phase clusters can be present inside the high-temperature filaments indicating that the filament structure is not uniform. Our results provide a unique perspective on the electrically induced filament formation in metal-insulator transition materials, which further the basic understanding of this resistive switching., Comment: 29 pages, 10 figures; 19 pages main text, 3 figures; 10 pages Supplementary material, 7 figures

Hund's metals are multi-orbital systems with $3d$ or $4d$ electrons exhibiting both itinerant character and local moments, and they feature Kondo-like screenings of local orbital and spin moments, with suppressed coherence temperature driven by Hund's coupling $J_H$. They often exhibit magnetic order at low temperature, but how the interaction between the Kondo-like screening and long-range magnetic order is manifested in the quasiparticle spectrum remains an open question. Here we present spectroscopic signature of such interaction in a Hund's metal candidate MnSi exhibiting weak ferromagnetism. Our photoemission measurements reveal renormalized quasiparticle bands near the Fermi level with strong momentum dependence: the ferromagnetism manifests through possibly exchange-split bands (Q1) below $T_C$ , while the spin/orbital screenings lead to gradual development of quasiparticles (Q2) upon cooling. Our results demonstrate how the characteristic spin/orbital coherence in a Hund's metal could coexist and compete with the magnetic order to form a weak itinerant ferromagnet, via quasiparticle bands that are well separated in momentum space and exhibit distinct temperature dependence. Our results imply that the competition between the spin/orbital screening and the magnetic order in a Hund's metal bears intriguing similarity to the Kondo lattice systems., Comment: accepted by PRB

The shape of 3$d$-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the $d_{x^2-y^2}$ orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu-$L_3$ and Pr-$M_5$ resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa$_2$Cu$_3$O$_{7}$, where the Pr $f$-electrons create a direct orbital bridge between CuO$_2$ planes. With this, we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.

The mechanism of unconventional superconductivity in correlated materials remains a great challenge in condensed matter physics. The recent discovery of superconductivity in infinite-layer nickelates, as analog to high-Tc cuprates, has opened a new route to tackle this challenge. By growing 8 nm Pr0.8Sr0.2NiO2 films on the (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate, we successfully raise the transition temperature Tc from 9 K in the widely studied SrTiO3-substrated nickelates into 15 K. By combining x-ray absorption spectroscopy with the first-principles and many-body simulations, we find a positive correlation between Tc and the pre-edge peak intensity, which can be attributed to the hybridization between Ni and O orbitals induced by the strain. Our result suggests that structural engineering can further enhance unconventional superconductivity, and the charge-transfer property plays a crucial role in the pairing strength., Comment: 8 pages, 4 figures

The discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni$^{1+}$ cations possess nominally the same 3$d^9$ configuration as Cu$^{2+}$ in cuprates, the electronic structure variances remain elusive. Here, we present a soft x-ray photoemission spectroscopy study on parent and doped infinite-layer Pr-nickelate thin films with a doped perovskite reference. By identifying the Ni character with resonant photoemission and comparison to density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge transfer energy $\Delta$ ~8 eV, confirming the Mott-Hubbard electronic structure in contrast to charge-transfer cuprates. Near the Fermi level ($E_F$), we observe a signature of occupied rare-earth states in the parent compound, which is consistent with a self-doping picture. Our results demonstrate a correlation between the superconducting transition temperature and the oxygen 2$p$ hybridization near $E_F$ when comparing hole-doped nickelates and cuprates., Comment: 28 pages, 10 figures

Identifying what broken symmetries are present in the cuprates has become a major area of research. Many authors have reported evidence for so-called "$Q \sim 0$" order that involves broken inversion, mirror, chiral, or time-reversal symmetry that is uniform in space. Not all these observations are well understood and new experimental probes are needed. Here we use resonant soft x-ray scattering (RSXS) to search for $Q \sim 0$ order in Bi$_{2.1}$Sr$_{1.9}$CaCu$_2$O$_{8+x}$ (Bi-2212) by measuring the region of a forbidden Bragg peak, $(0,0,3)$, which is normally extinguished by symmetry but may become allowed on resonance if valence band order is present. Using circularly polarized light, we found that this reflection becomes allowed on the Cu $L_3$ resonance for temperatures $T_c < T < T^\ast$, though remains absent in linear polarization and at other temperatures. This observation suggests the existence of spatially uniform valence band order near the pseudogap temperature. In addition, we observed periodic oscillations in the specular reflectivity from the sample surface that resemble thin film interference fringes, though no known film is present. These fringes are highly resonant, appear in all polarizations, and exhibit a period that depends on the location where the beam strikes the sample surface. We speculate that these fringes arise from interaction between some intrinsic valence band instability and extrinsic structural surface morphologies of the material. Our study supports the existence of some kind of $Q \sim 0$ broken symmetry state in Bi-2212 at intermediate temperatures, and calls for further study using a microfocused beam that could disentangle microscopic effects from macroscopic heterogeneities., Comment: 9 pages, 4 figures

The realization of four-fold anisotropic magnetoresistance (AMR) in novel 3d-5d heterostructures has boosted major efforts in antiferromagnetic spintronics. However, despite the potential of incorporating strong spin-orbit coupling, only small AMR signals have been detected thus far, prompting a search for new mechanisms to enhance the signal. In this study on CaMnO3/CaIrO3 heterostructures, we report a unique dual-four-fold symmetric 70% AMR; a signal two orders of magnitude larger than previously observed in similar systems. We find that one order is enhanced by tuning a large biaxial anisotropy through octahedral tilts of similar sense in the constituent layers, while the second order is triggered by a spin-flop transition in a nearly Mott-type phase. Dynamics between these two phenomena as evidenced by the step-like AMR and a superimposed biaxial-anisotropy-induced AMR capture a subtle interplay of pseudospin coupling with the lattice and external magnetic field. Our study shows that a combination of charge-transfer, interlayer coupling, and a spin-flop transition can yield a giant AMR relevant for sensing and antiferromagnetic memory applications.

Recently CMOS (complementary metal-oxide semiconductor) sensors have progressed to a point where they may offer improved performance in imaging x-ray detection compared to the CCDs often used in x-ray satellites. We demonstrate x-ray detection in the soft x-ray band (250-1700 eV) by a commercially available back-illuminated Sony IMX290LLR CMOS sensor using the Advanced Photon Source at the Argonne National Laboratory. While operating the device at room temperature, we measure energy resolutions (FWHM) of 48 eV at 250 eV and 83 eV at 1700 eV which are comparable to the performance of the Chandra ACIS and the Suzaku XIS. Furthermore, we demonstrate that the IMX290LLR can withstand radiation up to 17.1 krad, making it suitable for use on spacecraft in low earth orbit.

Electronic correlations are crucial to the low energy physics of metallic systems with localized $d$ and $f$ states; however, their effect on band insulators and semiconductors is typically negligible. Here, we measure the electronic structure of the half-Heusler compound FeVSb, a band insulator with filled shell configuration of 18 valence electrons per formula unit ($s^2 p^6 d^{10}$). Angle-resolved photoemission spectroscopy (ARPES) reveals a mass renormalization of $m^{*}/m_{bare}= 1.4$, where $m^{*}$ is the measured effective mass and $m_{bare}$ is the mass from density functional theory (DFT) calculations with no added on-site Coulomb repulsion. Our measurements are in quantitative agreement with dynamical mean field theory (DMFT) calculations, highlighting the many-body origin of the mass renormalization. This mass renormalization lies in dramatic contrast to other filled shell intermetallics, including the thermoelectric materials CoTiSb and NiTiSn; and has a similar origin to that in FeSi, where Hund's coupling induced fluctuations across the gap can explain a dynamical self-energy and correlations. Our work calls for a re-thinking of the role of correlations and Hund's coupling in intermetallic band insulators.

New developments in the field of topological matter are often driven by materials discovery, including novel topological insulators, Dirac semimetals and Weyl semimetals. In the last few years, large efforts have been performed to classify all known inorganic materials with respect to their topology. Unfortunately, a large number of topological materials suffer from non-ideal band structures. For example, topological bands are frequently convoluted with trivial ones, and band structure features of interest can appear far below the Fermi level. This leaves just a handful of materials that are intensively studied. Finding strategies to design new topological materials is a solution. Here we introduce a new mechanism that is based on charge density waves and non-symmorphic symmetry to design an idealized Dirac semimetal. We then show experimentally that the antiferromagnetic compound GdSb$_{0.46}$Te$_{1.48}$ is a nearly ideal Dirac semimetal based on the proposed mechanism, meaning that most interfering bands at the Fermi level are suppressed. Its highly unusual transport behavior points to a thus far unknown regime, in which Dirac carriers with Fermi energy very close to the node seem to gradually localize in the presence of lattice and magnetic disorder.

Polar metals are an intriguing class of materials that simultaneously host free carriers and polar structural distortions. Despite the name "polar metal," however, most well-studied polar metals are poor electrical conductors. Here, we demonstrate the molecular beam epitaxial (MBE) growth of LaPtSb and LaAuGe, two polar metal compounds whose electrical resistivity is an order of magnitude lower than the well studied oxide polar metals. These materials belong to a broad family of $ABC$ intermetallics adopting the stuffed wurtzite structure, also known as hexagonal Heusler compounds. Scanning transmission electron microscopy (STEM) reveals a polar structure with unidirectionally buckled $BC$ (PtSb, AuGe) planes. Magnetotransport measurements demonstrate good metallic behavior with low residual resistivity ($\rho_{LaAuGe}=59.05$ $\mu\Omega\cdot$cm and $\rho_{LaAPtSb}=27.81$ $\mu\Omega\cdot$cm at 2K) and high carrier density ($n_h\sim 10^{21}$ cm$^{-3}$). Photoemission spectroscopy measurements confirm the band metallicity and are in quantitative agreement with density functional theory (DFT) calculations. Through DFT-Chemical Pressure and Crystal Orbital Hamilton Population analyses, the atomic packing factor is found to support the polar buckling of the structure, though the degree of direct interlayer $B-C$ bonding is limited by repulsion at the $A-C$ contacts. When combined with insulating hexagonal Heuslers, these materials provide a new platform for fully epitaxial, multiferroic heterostructures.

Resonant soft x-ray scattering (RSXS) is a leading probe of valence band order in materials best known for detecting charge density wave order in the copper-oxide superconductors. One of the biggest limitations on the RSXS technique is the presence of a severe fluorescence background which, like the RSXS cross section itself, is enhanced under resonant conditions. This background prevents the study of weak signals such as diffuse scattering from glassy or fluctuating order that is spread widely over momentum space. Recent advances in superconducting transition edge sensor (TES) detectors have led to major improvements in energy resolution and detection efficiency in the soft x-ray range. Here, we perform a RSXS study of stripe-ordered La$_{2-x}$Ba$_x$CuO$_4$ at the Cu $L_{3/2}$ edge (932.2 eV) using a TES detector with 1.5 eV resolution, to evaluate its utility for mitigating the fluorescence background problem. We find that, for suitable degree of detuning from the resonance, the TES rejects the fluorescence background, leading to a 5 to 10 times improvement in the statistical quality of the data compared to an equivalent, energy-integrated measurement. We conclude that a TES presents a promising approach to reducing background in RSXS studies and may lead to new discoveries in materials exhibiting valence band order that is fluctuating or glassy., Comment: 10 pages, 6 figures

Using angle-resolved photoemission spectroscopy (ARPES) and resonant ARPES, we report evidence of strong anisotropic conduction-f electron mixing (c-f mixing) in CeBi by observing a largely expanded Ce-5d pocket at low temperature, with no change in the Bi-6p bands. The Fermi surface (FS) expansion is accompanied by a pronounced spectral weight transfer from the local 4f 0 peak of Ce (corresponding to Ce3+) to the itinerant conduction bands near the Fermi level. Careful analysis suggests that the observed large FS change (with a volume expansion of the electron pocket up to 40%) can most naturally be explained by a small valence change (~ 1%) of Ce, which coexists with a very weak Kondo screening. Our work therefore provides evidence for a FS change driven by real charge fluctuations deep in the Kondo limit, which is made possible by the low carrier density., Comment: 3 figures

Magnetic van der Waals (vdW) materials have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far magnetic vdW materials are mainly insulating or semiconducting, and none of them possesses a high electronic mobility - a property that is rare in layered vdW materials in general. The realization of a magnetic high-mobility vdW material would open the possibility for novel magnetic twistronic or spintronic devices. Here we report very high carrier mobility in the layered vdW antiferromagnet GdTe3. The electron mobility is beyond 60,000 cm2 V-1 s-1, which is the highest among all known layered magnetic materials, to the best of our knowledge. Among all known vdW materials, the mobility of bulk GdTe3 is comparable to that of black phosphorus, and is only surpassed by graphite. By mechanical exfoliation, we further demonstrate that GdTe3 can be exfoliated to ultrathin flakes of three monolayers, and that the magnetic order and relatively high mobility is retained in approximately 20-nm-thin flakes.

We report the molecular beam epitaxial growth, structure, and electronic measurements of single-crystalline LaAuSb films on Al$_2$O$_3$ (0001) substrates. LaAuSb belongs to a broad family of hexagonal $ABC$ intermetallics in which the magnitude and sign of layer buckling have strong effects on properties, e.g., predicted hyperferroelecticity, polar metallicity, and Weyl and Dirac states. Scanning transmission electron microscopy reveals highly buckled planes of Au-Sb atoms, with strong interlayer Au-Au interactions and a doubling of the unit cell. This buckling is four times larger than the buckling observed in other $ABC$s with similar composition, e.g. LaAuGe and LaPtSb. Photoemission spectroscopy measurements and comparison with theory suggest an electronic driving force for the Au-Au dimerization, since LaAuSb, with a 19-electron count, has one more valence electron per formula unit than most stable $ABC$s. Our results suggest that the electron count, in addition to conventional parameters such as epitaxial strain and chemical pressure, provides a powerful means for tuning the layer buckling in ferroic $ABC$s., Comment: in press

In some metals containing a sub-lattice of rare earth or actinide ions, free local $f$ spins at high temperatures dissolve into the sea of quantum conduction electrons at low temperatures, where they become mobile excitations. Once mobile, the spins acquire charge, forming electrons of heavy mass, known as heavy fermions. In turn, the incorporation of heavy charges into the conduction sea leads to an increase in the volume of the Fermi surface. This process, called Kondo scattering, is accompanied by a dramatic, temperature dependent transformation of the electronic interactions and masses. Since the Kondo phenomena is controlled by quantum fluctuations, here we ask, at which point does the Fermi surface change character? A priori, the answer is not clear, since near its onset, the Kondo effect cannot be described as a simple hybridization of electronic eigenstates. Conventional descriptions of this Kondo scattering process consider that hybridization, Fermi volume change, and $f$-electron mobility occur simultaneously. However, using angle resolved photoemission spectroscopy to measure the evolution of excitations, we find that the changes of the Fermi surface emerge at temperatures an order of magnitude higher than the opening of the hybridization gap, and two orders of magnitude higher than the onset of the coherent character of the $f$-electrons. We suggest that the large changes in Fermi volume, driven by electronic fluctuations, occur at temperatures where the various $\Gamma_x \to \Gamma_y$ crystal field-split $f$ levels become accessible to conduction states of the corresponding symmetries. The separation of these energy scales significantly modifies the conventional description of the Kondo lattice effect, which still lacks a full theoretical description., Comment: Manuscript originally submitted to a peer-reviewed journal on February 27, 2015; please contact corresponding author for more details

We investigate the electronic structure of the epitaxial VO$_2$ films in the rutile phase using the density functional theory combined with the slave spin method (DFT+SS). In DFT-SS, the multiorbital Hubbard interactions are added to a DFT-fit tight-binding model, and we employ the slave-spin method to treat the electron correlation. We find that while stretching the system along the rutile $c$-axis results in a band structure favoring an anisotropic orbital fillings, the electron correlation favors an equal electron filling among $t_{2g}$ orbitals. These two distinct effects cooperatively induce interesting orbital-dependent redistributions of the electron occupations and the spectral weights, which pushes the strained VO$_2$ toward an orbital selective Mott transition (OSMT). The simulated single-particle spectral functions are directly compared to V L-edge resonant X-ray photoemission spectroscopy of epitaxial 10 nm VO$_2$/TiO$_2$ (001) and (100) strain orientations. Excellent agreement is observed between the simulations and experimental data regarding the strain-induced evolution of the lower Hubbard band. Simulations of rutile NbO$_2$ under similar strain conditions as VO$_2$ are performed, and we predict that OSMT will not occur in rutile NbO$_2$. Our results indicates that the electron correlation in VO$_2$ is important and can be modulated even in the rutile phase before the Peierls instability sets in., Comment: 8 pages, 9 figures, invited paper for Special Topic: Strain Engineering in Functional Materials by Journal of Applied Physics

In this work, we present a model of the surface states of nonsymmorphic semimetals. These are derived from surface mass terms that lift the high degeneracy imposed in the band structure by the nonsymmorphic bulk symmetries. Reflecting the reduced symmetry at the surface, the bulk bands are strongly modified. This leads to the creation of two-dimensional floating bands, which are distinct from Shockley states, quantum well states or topologically protected surface states. We focus on the layered semimetal ZrSiS to clarify the origin of its surface states. We demonstrate an excellent agreement between DFT calculations and ARPES measurements and present an effective four-band model in which similar surface bands appear. Finally, we emphasize the role of the surface chemical potential by comparing the surface density of states in samples with and without potassium coating. Our findings can be extended to related compounds and generalized to other crystals with nonsymmorphic symmetries., Comment: 8 pages, 5 figures