Light-element and purely charge-based topological materials.

We examine a class of Hamiltonians characterized by interatomic, interorbital even-odd parity hybridization as a model for a family of topological insulators without the need for spin-orbit coupling. Non-trivial properties of these materials are exemplified by studying the topologically-protected edge states of-hybridized alkali and alkaline earth atoms in one and two-dimensional lattices. In 1D the topological features are analogous to the canonical Su-Schrieffer-Heeger model but, remarkably, occur in the absence of dimerization.

Entropy Engineering and Tunable Magnetic Order in the Spinel High-Entropy Oxide.

Spinel oxides are an ideal setting to explore the interplay between configurational entropy, site selectivity, and magnetism in high-entropy oxides (HEOs). In this work, we characterize the magnetic properties of the spinel (Cr, Mn, Fe, Co, Ni)O and study the evolution of its magnetism as a function of nonmagnetic gallium substitution. Across the range of compositions studied here, from 0 to 40% Ga, magnetic susceptibility and powder neutron diffraction measurements show that ferrimagnetic order is robust in the spinel HEO.

High-order replica bands in monolayer FeSe/SrTiO revealed by polarization-dependent photoemission spectroscopy.

The mechanism of the enhanced superconductivity in monolayer FeSe/SrTiO has been enthusiastically studied and debated over the past decade. One specific observation has been taken to be of central importance: the replica bands in the photoemission spectrum. Although suggestive of electron-phonon interaction in the material, the essence of these spectroscopic features remains highly controversial.

Single-crystalline epitaxial TiO film: A metal and superconductor, similar to Ti metal.

Titanium monoxide (TiO), an important member of the rock salt 3d transition-metal monoxides, has not been studied in the stoichiometric single-crystal form. It has been challenging to prepare stoichiometric TiO due to the highly reactive Ti We adapt a closely lattice-matched MgO(001) substrate and report the successful growth of single-crystalline TiO(001) film using molecular beam epitaxy. This enables a first-time study of stoichiometric TiO thin films, showing that TiO is metal but in proximity to Mott insulating state.

Doping evolution of the Mott-Hubbard landscape in infinite-layer nickelates.

The recent observation of superconductivity in [Formula: see text] has raised fundamental questions about the hierarchy of the underlying electronic structure. Calculations suggest that this system falls in the Mott-Hubbard regime, rather than the charge-transfer configuration of other nickel oxides and the superconducting cuprates. Here, we use state-of-the-art, locally resolved electron energy-loss spectroscopy to directly probe the Mott-Hubbard character of [Formula: see text] Upon doping, we observe emergent hybridization reminiscent of the Zhang-Rice singlet via the oxygen-projected states, modification of the Nd 5d states, and the systematic evolution of Ni 3d hybridization and filling.

Critical Nature of the Ni Spin State in Doped NdNiO_{2}.

Superconductivity with T_{c}≈15  K was recently found in doped NdNiO_{2}. The Ni^{1+}O_{2} layers are expected to be Mott insulators, so hole doping should produce Ni^{2+} with S=1, incompatible with robust superconductivity. We show that the NiO_{2} layers fall inside a critical region where the large pd hybridization favors a singlet ^{1}A_{1} hole-doped state like in CuO_{2}.

Graphene-based bidirectional radiative thermal transfer method for heat engines.

We present a method for substantially enhancing the rate of heat transfer into and out of the working fluid of a heat engine, using bidirectional thermal radiation exchange between the external environment and many individual graphene layers that are dispersed and suspended within an inert gas. This hybrid working fluid has the unique composite property of high optical absorption/emission yet low specific heat. Consequently, it can heat and cool rapidly, enabling a much greater cycle frequency and a commensurate increase in specific power, in comparison to conventional closed-cycle heat engines for which the cycle frequency is limited by the use of slower, non-radiative, thermal transfer.

Metal-insulator-transition engineering by modulation tilt-control in perovskite nickelates for room temperature optical switching.

In transition metal perovskites ABO, the physical properties are largely driven by the rotations of the BO octahedra, which can be tuned in thin films through strain and dimensionality control. However, both approaches have fundamental and practical limitations due to discrete and indirect variations in bond angles, bond lengths, and film symmetry by using commercially available substrates. Here, we introduce modulation tilt control as an approach to tune the ground state of perovskite oxide thin films by acting explicitly on the oxygen octahedra rotation modes-that is, directly on the bond angles.

Electron Phonon Coupling versus Photoelectron Energy Loss at the Origin of Replica Bands in Photoemission of FeSe on SrTiO_{3}.

The recent observation of replica bands in single-layer FeSe/SrTiO_{3} by angle-resolved photoemission spectroscopy (ARPES) has triggered intense discussions concerning the potential influence of the FeSe electrons coupling with substrate phonons on the superconducting transition temperature. Here we provide strong evidence that the replica bands observed in the single-layer FeSe/SrTiO_{3} system and several other cases are largely due to the energy loss processes of the escaping photoelectron, resulted from the well-known strong coupling of external propagating electrons to Fuchs-Kliewer surface phonons in ionic materials in general. The photoelectron energy loss in ARPES on single-layer FeSe/SrTiO_{3} is calculated using the demonstrated successful semiclassical dielectric theory in describing low energy electron energy loss spectroscopy of ionic insulators.

Type-II Dirac semimetal stabilized by electron-phonon coupling.

There is major interest, in condensed matter physics, in understanding the role of topology: remarkable progress has been made in classifying topological properties of non-interacting electrons, and on understanding the interplay between topology and electron-electron interactions. We extend such studies to interactions with the lattice, and predict non-trivial topological effects in infinitely long-lived polaron bands. Specifically, for a two-dimensional many-band model with realistic electron-phonon coupling, we verify that sharp level crossings are possible for polaron eigenstates, and prove that they are responsible for a novel type of sharp transition in the ground state of the polaron that can occur at a fixed momentum.

Tuning the Two-Dimensional Electron Liquid at Oxide Interfaces by Buffer-Layer-Engineered Redox Reactions.

Polar discontinuities and redox reactions provide alternative paths to create two-dimensional electron liquids (2DELs) at oxide interfaces. Herein, we report high mobility 2DELs at interfaces involving SrTiO (STO) achieved using polar LaSrMnO (LSMO) buffer layers to manipulate both polarities and redox reactions from disordered overlayers grown at room temperature. Using resonant X-ray reflectometry experiments, we quantify redox reactions from oxide overlayers on STO as well as polarity induced electronic reconstruction at epitaxial LSMO/STO interfaces.

Ground-state oxygen holes and the metal-insulator transition in the negative charge-transfer rare-earth nickelates.

The metal-insulator transition and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here we combine X-ray absorption and resonant inelastic X-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of rare-earth nickelates, taking NdNiO thin film as representative example.

Doping-dependent charge order correlations in electron-doped cuprates.

Understanding the interplay between charge order (CO) and other phenomena (for example, pseudogap, antiferromagnetism, and superconductivity) is one of the central questions in the cuprate high-temperature superconductors. The discovery that similar forms of CO exist in both hole- and electron-doped cuprates opened a path to determine what subset of the CO phenomenology is universal to all the cuprates. We use resonant x-ray scattering to measure the CO correlations in electron-doped cuprates (La2-x Ce x CuO4 and Nd2-x Ce x CuO4) and their relationship to antiferromagnetism, pseudogap, and superconductivity.

Real-space localization and quantification of hole distribution in chain-ladder Sr3Ca11Cu24O41 superconductor.

Understanding the physical properties of the chain-ladder Sr3Ca11Cu24O41 hole-doped superconductor has been precluded by the unknown hole distribution among chains and ladders. We use electron energy-loss spectrometry (EELS) in a scanning transmission electron microscope (STEM) at atomic resolution to directly separate the contributions of chains and ladders and to unravel the hole distribution from the atomic scale variations of the O-K near-edge structures. The experimental data unambiguously demonstrate that most of the holes lie within the chain layers.

Non-Zhang-Rice Singlet Character of the First Ionization State of T-CuO.

We argue that tetragonal CuO (T-CuO) has the potential to finally settle long-standing modeling issues for cuprate physics. We compare the one-hole quasiparticle (qp) dispersion of T-CuO to that of cuprates, in the framework of the strongly correlated (U_{dd}→∞) limit of the three-band Emery model. Unlike in CuO_{2}, magnetic frustration in T-CuO breaks the C_{4} rotational symmetry and leads to strong deviations from the Zhang-Rice singlet picture in parts of the reciprocal space.

Graphenylene Nanotubes.

A new type of carbon nanotube, based on the graphenylene motif, is investigated using density functional and tight-binding methods. Analogous to conventional graphene-based nanotubes, a two-dimensional graphenylene sheet can be "rolled" into a seamless cylinder in armchair, zigzag, or chiral orientations. The resulting nanotube can be described using the familiar (n,m) nomenclature and possesses 4-, 6-, and 12-membered rings, with three distinct bond lengths, indicating a nonuniform distribution of the electron density.

Photon-impenetrable, electron-permeable: the carbon nanotube forest as a medium for multiphoton thermal-photoemission.

Combining the photoelectric and thermionic mechanisms to generate free electrons has been of great interest since the early days of quantum physics as exemplified by the Fowler-DuBridge theory, and recently proposed for highly efficient solar conversion. We present experimental evidence of this combined effect over the entire range spanning room-temperature photoemission to thermionic emission. Remarkably, the optical stimulus alone is responsible for both heating and photoemission at the same time.

Charge ordering in the electron-doped superconductor Nd(2-x)Ce(x)CuO₄.

In cuprate high-temperature superconductors, an antiferromagnetic Mott insulating state can be destabilized toward unconventional superconductivity by either hole or electron doping. In hole-doped (p-type) cuprates, a charge ordering (CO) instability competes with superconductivity inside the pseudogap state. We report resonant x-ray scattering measurements that demonstrate the presence of charge ordering in the n-type cuprate Nd(2-x)Ce(x)CuO4 near optimal doping.

Element specific monolayer depth profiling.

The electronic phase behavior and functionality of interfaces and surfaces in complex materials are strongly correlated to chemical composition profiles, stoichiometry and intermixing. Here a novel analysis scheme for resonant X-ray reflectivity maps is introduced to determine such profiles, which is element specific and non-destructive, and which exhibits atomic-layer resolution and a probing depth of hundreds of nanometers.

Charge disproportionation without charge transfer in the rare-earth-element nickelates as a possible mechanism for the metal-insulator transition.

We study a model for the metal-insulator (M-I) transition in the rare-earth-element nickelates RNiO3, based upon a negative charge transfer energy and coupling to a rocksaltlike lattice distortion of the NiO6 octahedra. Using exact diagonalization and the Hartree-Fock approximation we demonstrate that electrons couple strongly to these distortions. For small distortions the system is metallic, with a ground state of predominantly d8L character, where L_ denotes a ligand hole.

Magnon-mediated interactions between fermions depend strongly on the lattice structure.

We propose two new methods to calculate exactly the spectrum of two spin-1/2 charge carriers moving in a ferromagnetic background, at zero temperature. We find that if the spins are located on a different sublattice than that on which the fermions move, magnon-mediated effective interactions are very strong and can bind the fermions into low-energy bipolarons with triplet character. This never happens in models where spins and charge carriers share the same lattice, whether they are in the same band or in different bands.

Strain-induced spin states in atomically ordered cobaltites.

Epitaxial strain imposed in complex oxide thin films by heteroepitaxy is recognized as a powerful tool for identifying new properties and exploring the vast potential of materials performance. A particular example is LaCoO(3), a zero spin, nonmagnetic material in the bulk, whose strong ferromagnetism in a thin film remains enigmatic despite a decade of intense research. Here, we use scanning transmission electron microscopy complemented by X-ray and optical spectroscopy to study LaCoO(3) epitaxial thin films under different strain states.

High-spin polaron in lightly doped CuO2 planes.

We derive and investigate numerically a minimal yet detailed spin-polaron model that describes lightly doped CuO2 layers. The low-energy physics of a hole is studied by total-spin-resolved exact diagonalization on clusters of up to 32 CuO2 unit cells, revealing features missed by previous studies. In particular, spin-polaron states with total spin 3/2 are the lowest eigenstates in some regions of the Brillouin zone.