Hydrogen-Driven Low-Temperature Topotactic Transition in Nanocomb Cobaltite for Ultralow Power Ionic-Magnetic Coupled Applications.

We reversibly control ferromagnetic-antiferromagnetic ordering in an insulating ground state by annealing tensile-strained LaCoO3 films in hydrogen. This ionic-magnetic coupling occurs due to the hydrogen-driven topotactic transition between perovskite LaCoO3 and brownmillerite La2Co2O5 at a lower temperature (125-200 °C) and within a shorter time (3-10 min) than the oxygen-driven effect (500 °C, tens of hours). The X-ray and optical spectroscopic analyses reveal that the transition results from hydrogen-driven filling of correlated electrons in the Co 3d-orbitals, which successively releases oxygen by destabilizing the CoO6 octahedra into CoO4 tetrahedra. The transition is accelerated by surface exchange, diffusion of hydrogen in and oxygen out through atomically ordered oxygen vacancy "nanocomb" stripes in the tensile-strained LaCoO3 films. Our ionic-magnetic coupling with fast operation, good reproducibility, and long-term stability is a proof-of-principle demonstration of high-performance ultralow power magnetic switching devices for sensors, energy, and artificial intelligence applications, which are keys for attaining carbon neutrality.

Tuning orbital-selective phase transitions in a two-dimensional Hund's correlated system.

Hund's rule coupling (J) has attracted much attention recently for its role in the description of the novel quantum phases of multi-orbital materials. Depending on the orbital occupancy, J can lead to various intriguing phases. However, experimental confirmation of the orbital occupancy dependency has been difficult as controlling the orbital degrees of freedom normally accompanies chemical inhomogeneities. Here, we demonstrate a method to investigate the role of orbital occupancy in J related phenomena without inducing inhomogeneities. By growing SrRuO3 monolayers on various substrates with symmetry-preserving interlayers, we gradually tune the crystal field splitting and thus the orbital degeneracy of the Ru t2g orbitals. It effectively varies the orbital occupancies of two-dimensional (2D) ruthenates. Via in-situ angle-resolved photoemission spectroscopy, we observe a progressive metal-insulator transition (MIT). It is found that the MIT occurs with orbital differentiation: concurrent opening of a band insulating gap in the dxy band and a Mott gap in the dxz/yz bands. Our study provides an effective experimental method for investigation of orbital-selective phenomena in multi-orbital materials.

Heteroepitaxial Control of Fermi Liquid, Hund Metal, and Mott Insulator Phases in Single-Atomic-Layer Ruthenates.

Interfaces between dissimilar correlated oxides can offer devices with versatile functionalities, and great efforts have been made to manipulate interfacial electronic phases. However, realizing such phases is often hampered by the inability to directly access the electronic structure information; most correlated interfacial phenomena appear within a few atomic layers from the interface. Here, atomic-scale epitaxy and photoemission spectroscopy are utilized to realize the interface control of correlated electronic phases in atomic-scale ruthenate-titanate heterostructures. While bulk SrRuO3 is a ferromagnetic metal, the heterointerfaces exclusively generate three distinct correlated phases in the single-atomic-layer limit. The theoretical analysis reveals that atomic-scale structural proximity effects yield Fermi liquid, Hund metal, and Mott insulator phases in the quantum-confined SrRuO3 . These results highlight the extensive interfacial tunability of electronic phases, hitherto hidden in the atomically thin correlated heterostructure. Moreover, this experimental platform suggests a way to control interfacial electronic phases of various correlated materials.

Ultra-flat and long-lived plasmons in a strongly correlated oxide.

Plasmons in strongly correlated systems are attracting considerable attention due to their unconventional behavior caused by electronic correlation effects. Recently, flat plasmons with nearly dispersionless frequency-wave vector relations have drawn significant interest because of their intriguing physical origin and promising applications. However, these flat plasmons exist primarily in low-dimensional materials with limited wave vector magnitudes (q < ~0.7 Å-1). Here, we show that long-lived flat plasmons can propagate up to ~1.2 Å-1 in α-Ti2O3, a strongly correlated three-dimensional Mott-insulator, with an ultra-small energy fluctuation (<40 meV). The strong correlation effect renormalizes the electronic bands near Fermi level with a small bandwidth, which is responsible for the flat plasmons in α-Ti2O3. Moreover, these flat plasmons are not affected by Landau damping over a wide range of wave vectors (q < ~1.2 Å-1) due to symmetry constrains on the electron wavefunctions. Our work provides a strategy for exploring flat plasmons in strongly correlated systems, which in turn may give rise to novel plasmonic devices in which flat and long-lived plasmons are desirable.

Infrared Transparent and Electromagnetic Shielding Correlated Metals via Lattice-Orbital-Charge Coupling.

Despite being a requisite for modern transparent electronics, few metals have a sufficiently high infrared transmittance due to the free electron response. Here, upon alloying the correlated metal SrVO3 with BaVO3, the medium wavelength infrared transmittance at a wavelength of 4 µm is found to be 50% higher than those for Sn-doped In2O3 (ITO) and La-doped BaSnO3 (BLSO). The room temperature resistivity of the alloy of ∼100 µΩ cm is 1 order of magnitude lower than those of ITO and BLSO, guaranteeing a profound electromagnetic shielding effectiveness of 22-31 dB at 10 GHz in the X-band. Systematic investigations reveal symmetry breaking of VO6 oxygen octahedra in SrVO3 due to the substitution of Sr2+ with larger Ba2+ ions, localization of electrons in the lower energy V-dyz and dzx orbitals, and stronger correlation effects. The lattice-orbital-charge-coupled engineering of the electronic band structure in correlated metals offers a new design strategy to create super-broad-band transparent conductors with an enhanced shielding capability.

Bulk Metamaterials Exhibiting Chemically Tunable Hyperbolic Responses.

Extraordinary properties of traditional hyperbolic metamaterials, not found in nature, arise from their man-made subwavelength structures causing unique light-matter interactions. However, their preparation requiring nanofabrication processes is highly challenging and merely provides nanoscale two-dimensional structures. Stabilizing their bulk forms via scalable procedures has been a sought-goal for broad applications of this technology. Herein, we report a new strategy of designing and realizing bulk metamaterials with finely tunable hyperbolic responses. We develop a facile two-step process: (1) self-assembly to obtain heterostructured nanohybrids of building blocks and (2) consolidation to convert nanohybrid powders to dense bulk pellets. Our samples have centimeter-scale dimensions typically, readily further scalable. Importantly, the thickness of building blocks and their relative concentration in bulk materials serve as a delicate means of controlling hyperbolic responses. The resulting new bulk heterostructured material system consists of the alternating h-BN and graphite/graphene nanolayers and exhibits significant modulation in both type-I and type-II hyperbolic resonance modes. It is the first example of real bulk hyperbolic metamaterials, consequently displaying the capability of tuning their responses along both in-plane and out-of-plane directions of the materials for the first time. It also distinctly interacts with unpolarized and polarized transverse magnetic and electronic beams to give unique hyperbolic responses. Our achievement can be a new platform to create various bulk metamaterials without complicated nanofabrication techniques. Our facile synthesis method using common laboratory techniques can open doors to broad-range researchers for active interdisciplinary studies for this otherwise hardly accessible technology.

Correlated Magnetic Weyl Semimetal State in Strained Pr2 Ir2 O7.

Correlated topological phases (CTPs) with interplay between topology and electronic correlations have attracted tremendous interest in condensed matter physics. Therein, correlated Weyl semimetals (WSMs) are rare in nature and, thus, have so far been less investigated experimentally. In particular, the experimental realization of the interacting WSM state with logarithmic Fermi velocity renormalization has not been achieved yet. Here, experimental evidence of a correlated magnetic WSM state with logarithmic renormalization in strained pyrochlore iridate Pr2 Ir2 O7 (PIO) which is a paramagnetic Luttinger semimetal in bulk, is reported. Benefitting from epitaxial strain, "bulk-absent" all-in-all-out antiferromagnetic ordering can be stabilized in PIO film, which breaks time-reversal symmetry and leads to a magnetic WSM state. With further analysis of the experimental data and renormalization group calculations, an interacting Weyl liquid state with logarithmically renormalized Fermi velocity, similar to that in graphene, is found, dressed by long-range Coulomb interactions. This work highlights the interplay of strain, magnetism, and topology with electronic correlations, and paves the way for strain-engineering of CTPs in pyrochlore iridates.

Topological Magnon Band Crossing in Y_{2}Ir_{2}O_{7}.

Topological magnonic materials have attracted much interest because of the potential for dissipationless spintronic applications. Pyrochlore iridates are theoretically regarded as good candidates for designing topological magnon bands. However, experimental identification of topological magnon bands in pyrochlore iridates remains elusive. We explored this possibility in Y_{2}Ir_{2}O_{7} using Raman spectroscopy to measure both the single-magnon excitations and anomalous phonon shifts. From the single-magnon energies and tight-binding model calculations concerning the phonons, we determined the key parameters in the spin Hamiltonian. These confirm that Y_{2}Ir_{2}O_{7} hosts a nontrivial magnon band topology distinct from other pyrochlore iridate compounds. Our work demonstrates that pyrochlore iridates constitute a system in which the magnon band topology can be tailored and that Raman spectroscopy is a powerful technique to explore magnon band topology.

Strain engineering of the magnetic multipole moments and anomalous Hall effect in pyrochlore iridate thin films.

The recent observation of the anomalous Hall effect (AHE) without notable magnetization in antiferromagnets has suggested that ferromagnetic ordering is not a necessary condition. Thus, recent theoretical studies have proposed that higher-rank magnetic multipoles formed by clusters of spins (cluster multipoles) can generate the AHE without magnetization. Despite such an intriguing proposal, controlling the unconventional AHE by inducing these cluster multipoles has not been investigated. Here, we demonstrate that strain can manipulate the hidden Berry curvature effect by inducing the higher-rank cluster multipoles in spin-orbit-coupled antiferromagnets. Observing the large AHE on fully strained antiferromagnetic Nd2Ir2O7 thin films, we prove that strain-induced cluster T 1-octupoles are the only source of observed AHE. Our results provide a previously unidentified pathway for generating the unconventional AHE via strain-induced magnetic structures and establish a platform for exploring undiscovered topological phenomena via strain in correlated materials.

Phase Instability amid Dimensional Crossover in Artificial Oxide Crystal.

Artificial crystals synthesized by atomic-scale epitaxy provide the ability to control the dimensions of the quantum phases and associated phase transitions via precise thickness modulation. In particular, the reduction in dimensionality via quantized control of atomic layers is a powerful approach to revealing hidden electronic and magnetic phases. Here, we demonstrate a dimensionality-controlled and induced metal-insulator transition (MIT) in atomically designed superlattices by synthesizing a genuine two-dimensional (2D) SrRuO_{3} crystal with highly suppressed charge transfer. The tendency to ferromagnetically align the spins in an SrRuO_{3} layer diminishes in 2D as the interlayer exchange interaction vanishes, accompanying the 2D localization of electrons. Furthermore, electronic and magnetic instabilities in the two SrRuO_{3} unit cell layers induce a thermally driven MIT along with a metamagnetic transition.

Charge-Spin Correlation in van der Waals Antiferromagnet NiPS_{3}.

Strong charge-spin coupling is found in a layered transition-metal trichalcogenide NiPS_{3}, a van der Waals antiferromagnet, from studies of the electronic structure using several experimental and theoretical tools: spectroscopic ellipsometry, x-ray absorption, photoemission spectroscopy, and density functional calculations. NiPS_{3} displays an anomalous shift in the optical spectral weight at the magnetic ordering temperature, reflecting strong coupling between the electronic and magnetic structures. X-ray absorption, photoemission, and optical spectra support a self-doped ground state in NiPS_{3}. Our work demonstrates that layered transition-metal trichalcogenide magnets are useful candidates for the study of correlated-electron physics in two-dimensional magnetic materials.