Interfacial charge-transfer Mott state in iridate-nickelate superlattices.

We investigate [Formula: see text]/[Formula: see text] superlattices in which we observe a full electron transfer at the interface from Ir to Ni, triggering a massive structural and electronic reconstruction. Through experimental characterization and first-principles calculations, we determine that a large crystal field splitting from the distorted interfacial [Formula: see text] octahedra surprisingly dominates over the spin-orbit coupling and together with the Hund's coupling results in the high-spin (S = 1) configurations on both the Ir and Ni sites. This demonstrates the power of interfacial charge transfer in coupling lattice, charge, orbital, and spin degrees of freedom, opening fresh avenues of investigation of quantum states in oxide superlattices.

Proximate Quantum Spin Liquid on Designer Lattice.

Complementary to bulk synthesis, here we propose a designer lattice with extremely high magnetic frustration and demonstrate the possible realization of a quantum spin liquid state from both experiments and theoretical calculations. In an ultrathin (111) CoCr2O4 slice composed of three triangular and one kagome cation planes, the absence of a spin ordering or freezing transition is demonstrated down to 0.03 K, in the presence of strong antiferromagnetic correlations in the energy scale of 30 K between Co and Cr sublattices, leading to the frustration factor of ∼1000. Persisting spin fluctuations are observed at low temperatures via low-energy muon spin relaxation. Our calculations further demonstrate the emergence of highly degenerate magnetic ground states at the 0 K limit, due to the competition among multiply altered exchange interactions. These results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.

Magnetic Weyl Semimetallic Phase in Thin Films of Eu_{2}Ir_{2}O_{7}.

The interplay between electronic interactions and strong spin-orbit coupling is expected to create a plethora of fascinating correlated topological states of quantum matter. Of particular interest are magnetic Weyl semimetals originally proposed in the pyrochlore iridates, which are only expected to reveal their topological nature in thin film form. To date, however, direct experimental demonstrations of these exotic phases remain elusive, due to the lack of usable single crystals and the insufficient quality of available films. Here, we report on the discovery of signatures for the long-sought magnetic Weyl semimetallic phase in (111)-oriented Eu_{2}Ir_{2}O_{7} high-quality epitaxial thin films. We observed an intrinsic anomalous Hall effect with colossal coercivity but vanishing net magnetization, which emerges right below the onset of a peculiar magnetic phase with all-in-all-out (AIAO) antiferromagnetic ordering. The anomalous Hall conductivity obtained experimentally is consistent with the theoretical prediction, likely arising from the nonzero Berry curvature emanated by Weyl node pairs near the Fermi level that act as sources and sinks of Berry flux, activated by broken cubic crystal symmetry at the top and bottom terminations of the thin film.

Emergent Magnetic State in (111)-Oriented Quasi-Two-Dimensional Spinel Oxides.

We report on the emergent magnetic state of (111)-oriented CoCr2O4 ultrathin films sandwiched between Al2O3 spacer layers in a quantum confined geometry. At the two-dimensional crossover, polarized neutron reflectometry reveals an anomalous enhancement of the total magnetization compared to the bulk value. Synchrotron X-ray magnetic circular dichroism measurements demonstrate the appearance of a long-range ferromagnetic ordering of spins on both Co and Cr sublattices. Brillouin function analyses and ab-initio density functional theory calculations further corroborate that the observed phenomena are due to the strongly altered magnetic frustration invoked by quantum confinement effects, manifested by the onset of a Yafet-Kittel-type ordering as the magnetic ground state in the ultrathin limit, which is unattainable in the bulk.

Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3.

Artificial complex-oxide heterostructures containing ultrathin buried layers grown along the pseudocubic [111] direction have been predicted to host a plethora of exotic quantum states arising from the graphene-like lattice geometry and the interplay between strong electronic correlations and band topology. To date, however, electronic-structural investigations of such atomic layers remain an immense challenge due to the shortcomings of conventional surface-sensitive probes with typical information depths of a few angstroms. Here, we use a combination of bulk-sensitive soft X-ray angle-resolved photoelectron spectroscopy (SX-ARPES), hard X-ray photoelectron spectroscopy (HAXPES), and state-of-the-art first-principles calculations to demonstrate a direct and robust method for extracting momentum-resolved and angle-integrated valence-band electronic structure of an ultrathin buckled graphene-like layer of NdNiO3 confined between two 4-unit cell-thick layers of insulating LaAlO3. The momentum-resolved dispersion of the buried Ni d states near the Fermi level obtained via SX-ARPES is in excellent agreement with the first-principles calculations and establishes the realization of an antiferro-orbital order in this artificial lattice. The HAXPES measurements reveal the presence of a valence-band bandgap of 265 meV. Our findings open a promising avenue for designing and investigating quantum states of matter with exotic order and topology in a few buried layers.

Polar phase transitions in heteroepitaxial stabilized La0.5Y0.5AlO3 thin films.

We report on the fabrication of epitaxial La0.5Y0.5AlO3 ultrathin films on (001) LaAlO3 substrates. Structural characterizations by scanning transmission electron microscopy and x-ray diffraction confirm the high quality of the film with a - b + c - AlO6 octahedral tilt pattern. Unlike either of the nonpolar parent compound, LaAlO3 and YAlO3, second harmonic generation measurements on the thin films suggest a nonpolar-polar phase transition at T c near 500 K, and a polar-polar phase transition at T a near 160 K. By fitting the angular dependence of the second harmonic intensities, we further propose that the two polar structures can be assigned to the Pmc2 1 and Pmn2 1 space group, while the high temperature nonpolar structure belongs to the Pbnm space group.

Ramp-Reversal Memory and Phase-Boundary Scarring in Transition Metal Oxides.

Transition metal oxides are complex electronic systems that exhibit a multitude of collective phenomena. Two archetypal examples are VO2 and NdNiO3 , which undergo a metal-insulator phase transition (MIT), the origin of which is still under debate. Here this study reports the discovery of a memory effect in both systems, manifested through an increase of resistance at a specific temperature, which is set by reversing the temperature ramp from heating to cooling during the MIT. The characteristics of this ramp-reversal memory effect do not coincide with any previously reported history or memory effects in manganites, electron-glass or magnetic systems. From a broad range of experimental features, supported by theoretical modelling, it is found that the main ingredients for the effect to arise are the spatial phase separation of metallic and insulating regions during the MIT and the coupling of lattice strain to the local transition temperature of the phase transition. We conclude that the emergent memory effect originates from phase boundaries at the reversal temperature leaving "scars" in the underlying lattice structure, giving rise to a local increase in the transition temperature. The universality and robustness of the effect shed new light on the MIT in complex oxides.

Built-in Electric Field Induced Mechanical Property Change at the Lanthanum Nickelate/Nb-doped Strontium Titanate Interfaces.

The interactions between electric field and the mechanical properties of materials are important for the applications of microelectromechanical and nanoelectromechanical systems, but relatively unexplored for nanoscale materials. Here, we observe an apparent correlation between the change of the fractured topography of Nb-doped SrTiO3 (Nb:STO) within the presence of a built-in electric field resulting from the Schottky contact at the interface of a metallic LaNiO3 thin film utilizing cross-sectional scanning tunneling microscopy and spectroscopy. The change of the inter-atomic bond length mechanism is argued to be the most plausible origin. This picture is supported by the strong-electric-field-dependent permittivity in STO and the existence of the dielectric dead layer at the interfaces of STO with metallic films. These results provided direct evidence and a possible mechanism for the interplay between the electric field and the mechanical properties on the nanoscale for perovskite materials.

Visualizing short-range charge transfer at the interfaces between ferromagnetic and superconducting oxides.

The interplay between antagonistic superconductivity and ferromagnetism has been a interesting playground to explore the interaction between competing ground states. Although this effect in systems of conventional superconductors is better understood, the framework of the proximity effect at complex-oxide-based superconductor/ferromagnet interfaces is not so clear. The main difficulty originates from the lack of experimental tools capable of probing the interfaces directly with high spatial resolution. Here we harness cross-sectional scanning tunnelling microscopy and spectroscopy together with atomic-resolution electron microscopy to understand the buried interfaces between cuprate and manganite layers. The results show that the fundamental length scale of the electronic evolution between YBa2Cu3O(7-δ) (YBCO) and La2/3Ca1/3MnO3 (LCMO) is confined to the subnanometre range. Our findings provide a complete and direct microscopic picture of the electronic transition across the YBCO/LCMO interfaces, which is an important step towards understanding the competition between ferromagnetism and superconductivity in complex-oxide heterostructures.

Heterointerface engineered electronic and magnetic phases of NdNiO3 thin films.

Mott physics is characterized by an interaction-driven metal-to-insulator transition in a partially filled band. In the resulting insulating state, antiferromagnetic orders of the local moments typically develop, but in rare situations no long-range magnetic order appears, even at zero temperature, rendering the system a quantum spin liquid. A fundamental and technologically critical question is whether one can tune the underlying energetic landscape to control both metal-to-insulator and Néel transitions, and even stabilize latent metastable phases, ideally on a platform suitable for applications. Here we demonstrate how to achieve this in ultrathin films of NdNiO3 with various degrees of lattice mismatch, and report on the quantum critical behaviours not reported in the bulk by transport measurements and resonant X-ray spectroscopy/scattering. In particular, on the decay of the antiferromagnetic Mott insulating state into a non-Fermi liquid, we find evidence of a quantum metal-to-insulator transition that spans a non-magnetic insulating phase.