Tunable 2D Electron- and 2D Hole States Observed at Fe/SrTiO3 Interfaces.

Oxide electronics provide the key concepts and materials for enhancing silicon-based semiconductor technologies with novel functionalities. However, a basic but key property of semiconductor devices still needs to be unveiled in its oxidic counterparts: the ability to set or even switch between two types of carriers-either negatively (n) charged electrons or positively (p) charged holes. Here, direct evidence for individually emerging n- or p-type 2D band dispersions in STO-based heterostructures is provided using resonant photoelectron spectroscopy. The key to tuning the carrier character is the oxidation state of an adjacent Fe-based interface layer: For Fe and FeO, hole bands emerge in the empty bandgap region of STO due to hybridization of Ti- and Fe- derived states across the interface, while for Fe3O4 overlayers, an 2D electron system is formed. Unexpected oxygen vacancy characteristics arise for the hole-type interfaces, which as of yet had been exclusively assigned to the emergence of 2DESs. In general, this finding opens up the possibility to straightforwardly switch the type of conductivity at STO interfaces by the oxidation state of a redox overlayer. This will extend the spectrum of phenomena in oxide electronics, including the realization of combined n/p-type all-oxide transistors or logic gates.

Superconducting Instabilities in Strongly Correlated Infinite-Layer Nickelates.

The discovery of superconductivity in infinite-layer nickelates has added a new family of materials to the fascinating growing class of unconventional superconductors. By incorporating the strongly correlated multiorbital nature of the low-energy electronic degrees of freedom, we compute the leading superconducting instability from magnetic fluctuations relevant for infinite-layer nickelates. Specifically, by properly including the doping dependence of the Ni d_{x^{2}-y^{2}} and d_{z^{2}} orbitals as well as the self-doping band, we uncover a transition from d-wave pairing symmetry to nodal s_{±} superconductivity, driven by strong fluctuations in the d_{z^{2}}-dominated orbital states. We discuss the properties of the resulting superconducting condensates in light of recent tunneling and penetration depth experiments probing the detailed superconducting gap structure of these materials.

Unconventional Hund metal in a weak itinerant ferromagnet.

The physics of weak itinerant ferromagnets is challenging due to their small magnetic moments and the ambiguous role of local interactions governing their electronic properties, many of which violate Fermi-liquid theory. While magnetic fluctuations play an important role in the materials' unusual electronic states, the nature of these fluctuations and the paradigms through which they arise remain debated. Here we use inelastic neutron scattering to study magnetic fluctuations in the canonical weak itinerant ferromagnet MnSi. Data reveal that short-wavelength magnons continue to propagate until a mode crossing predicted for strongly interacting quasiparticles is reached, and the local susceptibility peaks at a coherence energy predicted for a correlated Hund metal by first-principles many-body theory. Scattering between electrons and orbital and spin fluctuations in MnSi can be understood at the local level to generate its non-Fermi liquid character. These results provide crucial insight into the role of interorbital Hund's exchange within the broader class of enigmatic multiband itinerant, weak ferromagnets.

Uncovering the Mechanism of the Impurity-Selective Mott Transition in Paramagnetic V_{2}O_{3}.

While the phase diagrams of the one- and multiorbital Hubbard model have been well studied, the physics of real Mott insulators is often much richer, material dependent, and poorly understood. In the prototype Mott insulator V_{2}O_{3}, chemical pressure was initially believed to explain why the paramagnetic-metal to antiferromagnetic-insulator transition temperature is lowered by Ti doping while Cr doping strengthens correlations, eventually rendering the high-temperature phase paramagnetic insulating. However, this scenario has been recently shown both experimentally and theoretically to be untenable. Based on full structural optimization, we demonstrate via the charge self-consistent combination of density functional theory and dynamical mean-field theory that changes in the V_{2}O_{3} phase diagram are driven by defect-induced local symmetry breakings resulting from dramatically different couplings of Cr and Ti dopants to the host system. This finding emphasizes the high sensitivity of the Mott metal-insulator transition to the local environment and the importance of accurately accounting for the one-electron Hamiltonian, since correlations crucially respond to it.

Orbital Ordering of the Mobile and Localized Electrons at Oxygen-Deficient LaAlO3/SrTiO3 Interfaces.

Interfacing different transition-metal oxides opens a route to functionalizing their rich interplay of electron, spin, orbital, and lattice degrees of freedom for electronic and spintronic devices. Electronic and magnetic properties of SrTiO3-based interfaces hosting a mobile two-dimensional electron system (2DES) are strongly influenced by oxygen vacancies, which form an electronic dichotomy, where strongly correlated localized electrons in the in-gap states (IGSs) coexist with noncorrelated delocalized 2DES. Here, we use resonant soft-X-ray photoelectron spectroscopy to prove the eg character of the IGSs, as opposed to the t2g character of the 2DES in the paradigmatic LaAlO3/SrTiO3 interface. We furthermore separate the d xy and d xz/d xz orbital contributions based on deeper consideration of the resonant photoexcitation process in terms of orbital and momentum selectivity. Supported by a self-consistent combination of density functional theory and dynamical mean field theory calculations, this experiment identifies local orbital reconstruction that goes beyond the conventional eg- vs-t2g band ordering. A hallmark of oxygen-deficient LaAlO3/SrTiO3 is a significant hybridization of the eg and t2g orbitals. Our findings provide routes for tuning the electronic and magnetic properties of oxide interfaces through "defect engineering" with oxygen vacancies.

Unconventional electron states in δ-doped SmTiO3.

The Mott-insulating distorted perovskite SmTiO3, doped with a single SrO layer in a quantum-well architecture is studied by the combination of density functional theory with dynamical mean-field theory. A rich correlated electronic structure in line with recent experimental investigations is revealed by the given realistic many-body approach to a large-unit-cell oxide heterostructure. Coexistence of conducting and Mott-insulating TiO2 layers prone to magnetic order gives rise to multi-orbital electronic transport beyond standard Fermi-liquid theory. First hints towards a pseudogap opening due to electron-electron scattering within a background of ferromagnetic and antiferromagnetic fluctuations are detected.

Magnetism, Spin Texture, and In-Gap States: Atomic Specialization at the Surface of Oxygen-Deficient SrTiO_{3}.

Motivated by recent spin- and angular-resolved photoemission (SARPES) measurements of the two-dimensional electronic states confined near the (001) surface of oxygen-deficient SrTiO_{3}, we explore their spin structure by means of ab initio density functional theory (DFT) calculations of slabs. Relativistic nonmagnetic DFT calculations display Rashba-like spin winding with a splitting of a few meV and when surface magnetism on the Ti ions is included, bands become spin-split with an energy difference ∼100 meV at the Γ point, consistent with SARPES findings. While magnetism tends to suppress the effects of the relativistic Rashba interaction, signatures of it are still clearly visible in terms of complex spin textures. Furthermore, we observe an atomic specialization phenomenon, namely, two types of electronic contributions: one is from Ti atoms neighboring the oxygen vacancies that acquire rather large magnetic moments and mostly create in-gap states; another comes from the partly polarized t_{2g} itinerant electrons of Ti atoms lying further away from the oxygen vacancy, which form the two-dimensional electron system and are responsible for the Rashba spin winding and the spin splitting at the Fermi surface.

Theoretical prediction of a strongly correlated Dirac metal.

Recently, the most intensely studied objects in the electronic theory of solids have been strongly correlated systems and graphene. However, the fact that the Dirac bands in graphene are made up of sp(2) electrons, which are subject to neither strong Hubbard repulsion U nor strong Hund's rule coupling J, creates certain limitations in terms of novel, interaction-induced physics that could be derived from Dirac points. Here we propose GaCu3(OH)6Cl2 (Ga-substituted herbertsmithite) as a correlated Dirac-Kagome metal combining Dirac electrons, strong interactions and frustrated magnetic interactions. Using density functional theory, we calculate its crystallographic and electronic properties, and observe that it has symmetry-protected Dirac points at the Fermi level. Its many-body physics is diverse, with possible charge, magnetic and superconducting instabilities. Through a combination of various many-body methods we study possible symmetry-lowering phase transitions such as Mott-Hubbard, charge or magnetic ordering, and unconventional superconductivity, which in this compound assumes an f-wave symmetry.

Strong correlations enhanced by charge ordering in highly doped cobaltates.

We present an explanation for the puzzling spectral and transport properties of layered cobaltates close to the band-insulator limit, which relies on the key effect of charge ordering. Blocking a significant fraction of the lattice sites deeply modifies the electronic structure in a way that is shown to be quantitatively consistent with photoemission experiments. It also makes the system highly sensitive to interactions (especially to intersite ones), hence accounting for the strong correlations effects observed in this regime, such as the high effective mass and quasiparticle scattering rate. These conclusions are supported by a theoretical study of an extended Hubbard model with a realistic band structure on an effective kagome lattice.

Detecting excitation and magnetization of individual dopants in a semiconductor.

An individual magnetic atom doped into a semiconductor is a promising building block for bottom-up spintronic devices and quantum logic gates. Moreover, it provides a perfect model system for the atomic-scale investigation of fundamental effects such as magnetism in dilute magnetic semiconductors. However, dopants in semiconductors so far have not been studied by magnetically sensitive techniques with atomic resolution that correlate the atomic structure with the dopant's magnetism. Here we show electrical excitation and read-out of a spin associated with a single magnetic dopant in a semiconductor host. We use spin-resolved scanning tunnelling spectroscopy to measure the spin excitations and the magnetization curve of individual iron surface-dopants embedded within a two-dimensional electron gas confined to an indium antimonide (110) surface. The dopants act like isolated quantum spins the states of which are governed by a substantial magnetic anisotropy that forces the spin to lie in the surface plane. This result is corroborated by our first principles calculations. The demonstrated methodology opens new routes for the investigation of sample systems that are more widely studied in the field of spintronics-that is, Mn in GaAs (ref. 5), magnetic ions in semiconductor quantum dots, nitrogen-vacancy centres in diamond and phosphorus spins in silicon.

Electronic correlations in vanadium chalcogenides: BaV Se(3) versus BaV S(3).

Albeit structurally and electronically very similar, at low temperature the quasi-one-dimensional vanadium sulfide BaV S(3) shows a metal-to-insulator transition via the appearance of a charge-density-wave state, while BaV Se(3) apparently remains metallic down to zero temperature. This different behavior upon cooling is studied by means of density functional theory and its combination with the dynamical mean-field theory and the rotationally invariant slave-boson method. We reveal several subtle differences between these chalcogenides that provide indications for the deviant behavior of BaV Se(3) at low temperature. In this regard, a smaller Hubbard U in line with an increased relevance of the Hund's exchange J plays a vital role.

Correlation effects on the doped triangular lattice in view of the physics of sodium-rich NaxCoO2.

The peculiar correlation effects on the triangular lattice are studied by means of the rotationally invariant slave boson method in a cellular cluster approach. Hence nonlocal correlations are included in a short-range regime. Their impact for the single-band Hubbard model is studied at half filling, i.e., on the Mott transition, and with doping. Using the realistic band structure of NaxCoO2, we may also shed light on the cobaltate physics for x > or = 1/3, with the in-plane transition from antiferromagnetic tendencies towards the onset of ferromagnetism for a finite Hubbard U.

Importance of interorbital charge transfers for the metal-to-insulator transition of BaVS3.

The underlying mechanism of the metal-to-insulator transition (MIT) in BaVS3 is investigated, using dynamical mean-field theory in combination with density functional theory. It is shown that correlation effects are responsible for a strong charge redistribution, which lowers the occupancy of the broader A(1g) band in favor of the narrower E(g) bands and thereby substantially modifies the Fermi surface. This resolves several discrepancies between band theory and the experimental findings, such as the observed value of the charge-density-wave ordering vector associated with the MIT, and the presence of local moments in the metallic phase.