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In magnetic pyrochlore materials, the interplay of spin-orbit coupling, electronic correlations, and geometrical frustration gives rise to exotic quantum phases, including topological semimetals and spin ice. While these phases have been observed in isolation, the interface-driven phenomena emerging from their interaction have never been realized previously. Here, we report on the discovery of interfacial electronic anisotropy and rotational symmetry breaking at a heterostructure consisting of the Weyl semimetal Eu2Ir2O7 and spin ice Dy2Ti2O7. Subjected to magnetic fields, we unveil a six-fold anisotropic transport response that is theoretically accounted by a Kondo-coupled heterointerface, where the spin ice's field-tuned magnetism induces electron scattering in the Weyl semimetal's topological Fermi-arc states. Furthermore, at elevated magnetic fields, we reveal a two-fold anisotropic response indicative of a new symmetry-broken many-body state. This discovery showcases the nascent potential of complex quantum architectures in search of emergent phenomena unreachable in bulk crystals.

The synthesis of stoichiometric and epitaxial pyrochlore iridate thin films presents significant challenges yet is critical for unlocking experimental access to novel topological and magnetic states. Towards this goal, we unveil an in-situ two-stage growth mechanism that facilitates the synthesis of high-quality oriented pyrochlore iridate thin films. The growth starts with the deposition of a pyrochlore titanate as an active iso-structural template, followed by the application of an in-situ solid phase epitaxy technique in the second stage to accomplish the formation of single crystalline, large-area films. This novel protocol ensures the preservation of stoichiometry and structural homogeneity, leading to a marked improvement in surface and interface qualities over previously reported methods. The success of this synthesis approach is attributed to the application of directional laser-heat annealing, which effectively reorganizes the continuous random network of ions into a crystalline structure, as evidenced by our comprehensive analysis of the growth kinetics. This new synthesis approach advances our understanding of pyrochlore iridate film fabrication and opens a new perspective for investigating their unique physical properties., Comment: 11 pages, 4 figures; supplementary materials (1 table, 6 figures)

The pyrochlore iridates have become ideal platforms to unravel fascinating correlated and topolog?ical phenomena that stem from the intricate interplay among strong spin-orbit coupling, electronic correlations, lattice with geometric frustration, and itinerancy of the 5d electrons. The all-in-all?out antiferromagnetic state, commonly considered as the magnetic ground state, can be dramatically altered in reduced dimensionality, leading to exotic or hidden quantum states inaccessible in bulk. Here, by means of magnetotransport, resonant elastic and inelastic x-ray scattering experiments, we discover an emergent quantum disordered state in (111) Y2Ir2O7 thin films (thickness less than 30 nm) per?sisting down to 5 K, characterized by dispersionless magnetic excitations. The anomalous Hall effect observed below an onset temperature near 135 K corroborates the presence of chiral short-range spin configurations expressed in non-zero scalar spin chirality, breaking the macroscopic time-reversal symmetry. The origin of this chiral state is ascribed to the restoration of magnetic frustration on the pyrochlore lattice in lower dimensionality, where the competing exchange interactions together with enhanced quantum fluctuations suppress any long-range order and trigger spin-liquid-like behavior with degenerate ground-state manifold.

A prime goal for this lecture is to provide a reader with a reasonably self-sufficient answer to the question of what interesting effects can happen if you join two dissimilar materials with correlated carriers to construct a sandwich with the interface across those layers. Through the lens of physical phenomena, we will delve into the design ideas that lead to the creation of new synthetic quantum materials with properties primarily governed by the interface., Comment: 31 pages 8 figures in color

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 the long-sought magnetic Weyl semi-metallic phase in (111)-oriented Eu$_2$Ir$_2$O$_7$ high-quality epitaxial thin films. The topological magnetic state shows an intrinsic anomalous Hall effect with colossal coercivity but vanishing net magnetization, which emerges below the onset of a peculiar magnetic phase with all-in-all-out antiferromagnetic ordering. The observed anomalous Hall conductivity arises from the non-zero 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.

Frustrated rare-earth pyrochlore titanates, Yb$_2$Ti$_2$O$_7$, and Tb$_2$Ti$_2$O$_7$ have been proposed as promising candidates to realize quantum spin ice (QSI). Multiple exotic quantum phases, including Coulombic ferromagnet, quantum valence-bond solid, and quadrupolar ordering, have been predicted to emerge in the QSI state upon application of a (111)-oriented external magnetic field. Here, we report on the primal successful layer-by-layer growth of ultra-thin films of frustrated quantum pyrochlores, R$_2$Ti$_2$O$_7$ (R = Er, Yb, and Tb), along the (111) direction. We confirm their high crystallinity and proper chemical composition by a combination of methods, including in-situ RHEED, x-ray diffraction, reciprocal space mapping, and x-ray photoelectron spectroscopy. The availability of large area (111)-oriented QSI structures with planar geometry offers a new complementary to the bulk platform to explore strain and magnetic field dependent properties in the quasi-2D limit.

AB$_2$O$_4$ normal spinels with a magnetic B site can host a variety of magnetic and orbital frustrations leading to spin-liquid phases and field-induced phase transitions. Here we report the first epitaxial growth of (111)-oriented MgCr$_2$O$_4$ thin films. By characterizing the structural and electronic properties of films grown along (001) and (111) directions, the influence of growth orientation has been studied. Despite distinctly different growth modes observed during deposition, the comprehensive characterization reveals no measurable disorder in the cation distribution nor multivalency issue for Cr ions in either orientation. Contrary to a naive expectation, the (111) stabilized films exhibit a smoother surface and a higher degree of crystallinity than (001)-oriented films. The preference in growth orientation is explained within the framework of heteroepitaxial stabilization in connection to a significantly lower (111) surface energy. These findings open broad opportunities in the fabrication of 2D kagome-triangular heterostructures with emergent magnetic behavior inaccessible in bulk crystals.

We highlight recent advances in the theory, materials fabrication, and experimental characterization of strongly correlated and topological states in [111] oriented transition metal oxide thin films and heterostructures, which are notoriously difficult to realize compared to their [001] oriented counterparts. We focus on two classes of complex oxides, with the chemical formula ABO3 and A2B2O7, where the B sites are occupied by an open-shell transition metal ion with a local moment, and the A sites are typically a rare earth. The [111] oriented quasi-two-dimensional lattices derived from these parent compound lattices can exhibit peculiar geometries and symmetries, namely, a buckled honeycomb lattice, as well as kagome and triangular lattices. These lattice motifs form the basis for emergent strongly correlated and topological states expressed in exotic magnetism, various forms of orbital ordering, topological insulators, topological semimetals, quantum anomalous Hall insulators, and quantum spin liquids. For transition metal ions with high atomic number, spin-orbit coupling plays a significant role and may give rise to additional topological features in the electronic band structure and in the spectrum of magnetic excitations. We conclude the Perspective by articulating open challenges and opportunities in this actively developing field.

GeCu$_2$O$_4$ is a high-pressure recoverable cuprate with a strongly tetragonally elongated spinel structure and magnetic lattice formed by $S=1/2$ CuO$_2$ linear chains with frustrated exchange interactions and exotic magnetic behavior. Here we report on the first stabilization of epitaxial thin films of GeCu$_2$O$_4$ on (001)-oriented MgAl$_2$O$_4$ substrate. Developed growth mode, surface morphology, crystal structure and copper valence state were characterized by \emph{in-situ} reflection high-energy electron diffraction, atomic force microscopy, X-ray reflectivity, X-ray diffraction and X-ray photoelectron spectroscopy. The availability of large single-crystalline GeCu$_2$O$_4$ thin films paves road to comprehensive investigation of physical properties including the puzzle of magnetism and multiferroicity in this peculiar compound., Comment: Material of this manuscript was united with arXiv:1907.07785

Understanding the crystal field splitting and orbital polarization in non-centrosymmetric systems such as ferroelectric materials is fundamentally important. In this study, taking BaTiO$_3$ (BTO) as a representative material we investigate titanium crystal field splitting and orbital polarization in non-centrosymmetric TiO$_6$ octahedra with resonant X-ray linear dichroism at Ti $L_{2,3}$-edge. The high-quality BaTiO$_3$ thin films were deposited on DyScO$_3$ (110) single crystal substrates in a layer-by-layer way by pulsed laser deposition. The reflection high-energy electron diffraction (RHEED) and element specific X-ray absorption spectroscopy (XAS) were performed to characterize the structural and electronic properties of the films. In sharp contrast to conventional crystal field splitting and orbital configuration ($d_{xz}$/$d_{yz}$ $<$ $d_{xy}$ $<$ $d_{3z^2-r^2}$ $<$ $d_{x^2-y^2}$ or $d_{xy}$ $<$ $d_{xz}$/$d_{yz}$ $<$ $d_{x^2-y^2}$ $<$ $d_{3z^2-r^2}$) according to Jahn-Teller effect, it is revealed that $d_{xz}$, $d_{yz}$, and $d_{xy}$ orbitals are nearly degenerate, whereas $d_{3z^2-r^2}$ and $d_{x^2-y^2}$ orbitals are split with an energy gap $\sim$ 100 meV in the epitaxial BTO films. The unexpected degenerate states $d_{xz}$/$d_{yz}$/$d_{xy}$ are coupled to Ti-O displacements resulting from competition between polar and Jahn-Teller distortions in non-centrosymmetric TiO$_6$ octhedra of BTO films. Our results provide a route to manipulate orbital degree of freedom by switching electric polarization in ferroelectric materials.

A notion of the Berry phase is a powerful means to unravel the non-trivial role of topology in various novel phenomena observed in chiral magnetic materials and structures. A celebrated example is the intrinsic anomalous Hall effect (AHE) driven by the non-vanishing Berry phase in the momentum space. As the AHE is highly dependent on details of the band structure near the Fermi edge, the Berry phase and AHE can be altered in thin films whose chemical potential is tunable by dimensionality and disorder. Here, we demonstrate that in ultrathin SrRuO$_3$ films the Berry phase can be effectively manipulated by the effects of disorder on the intrinsic Berry phase contribution to the AHE, which is corroborated by our numerically exact calculations. In addition, our findings provide ample experimental evidence for the superficial nature of the topological Hall effect attribution to the protected spin texture and instead lend strong support to the multi-channel AHE scenario in ultrathin SrRuO$_3$.

Frustrated magnets can host numerous exotic many-body quantum and topological phenomena. GeNi$_2$O$_4$ is a three dimensional $S=1$ frustrated magnet with an unusual two-stage transition to the two-dimensional antiferromagnetic ground state, while GeCu$_2$O$_4$ is a high-pressure phase with a strongly tetragonally elongated spinel structure and magnetic lattice formed by $S=1/2$ CuO$_2$ linear chains with frustrated exchange interactions and exotic magnetic behavior. Here we report on the first thin-film epitaxial stabilization of these two compounds. Developed growth mode, surface morphology, crystal structure and copper valence state were characterized by in-situ reflection high-energy electron diffraction, atomic force microscopy, X-ray reflectivity, X-ray diffraction, X-ray photoelectron spectroscopy and resonant X-ray absorption spectroscopy. Our results pave an alternative route to the comprehensive investigation of the puzzling magnetic properties of these compounds and exploration of novel emergent features driven by strain.

We investigate THz conductivity dynamics in NdNiO$_3$ and EuNiO$_3$ thin films following a photoinduced thermal quench into the metallic state and reveal a clear contrast between first- and second-order dynamics. While in EuNiO$_3$ the conductivity recovers exponentially, in NdNiO$_3$ the recovery is non-exponential and slower than a simple thermal model. Crucially, it is consistent with first-order dynamics and well-described by a 2d Avrami model, with supercooling leading to metastable phase coexistence. The large transients seen in our films are promising for fast electronic (and magnetic) switching applications., Comment: includes supplemental material

Almost all oxide two-dimensional electron gases are formed in SrTiO$_3$-based heterostructures and the study of non-SrTiO$_3$ systems is extremely rare. Here, we report the realization of a two-dimensional electron gas in a CaTiO$_3$-based heterostructure, CaTiO$_3$/LaTiO$_3$, grown epitaxially layer-by-layer on a NdGaO$_3$ (110) substrate via pulsed laser deposition. The high quality of the crystal and electronic structures are characterized by in-situ reflection high-energy electron diffraction, X-ray diffraction, and X-ray photoemission spectroscopy. Measurement of electrical transport validates the formation of a two-dimensional electron gas in the CaTiO$_3$/LaTiO$_3$ superlattice. It is revealed the room-temperature carrier mobility in CaTiO$_3$/LaTiO$_3$ is nearly 3 times higher than in CaTiO$_3$/YTiO$_3$, demonstrating the effect of TiO$_6$ octahedral tilts and rotations on carrier mobility of two-dimensional electron gases. Due to doped CaTiO$_3$ being an A-site polar metal, our results provide a new route to design novel A-site two-dimensional polar metals.

LiOsO3 is one of the first materials identified in a recent literature as a 'polar metal', a class of materials that are simultaneously noncentrosymmetric and metallic. In this work, the linear and nonlinear optical susceptibility of LiOsO3 is studied by means of ellipsometry and optical second harmonic generation (SHG). Strong optical birefringence is observed using spectroscopic ellipsometry. The nonlinear optical susceptibility extracted from SHG polarimetry reveals that the tensor components are of the same magnitude as in isostructural insulator LiNbO3, except the component along the polar axis d33, which is suppressed by an order of magnitude. Temperature-dependent SHG measurements in combination with Raman spectroscopy indicate a continuous order-disorder type polar phase transition at 140 K. Linear and nonlinear optical microscopy techniques reveal 109 deg/71 deg ferroelastic domain walls, like in other trigonal ferroelectrics. No 180 deg polar domain walls are observed to emerge across the phase transition., Comment: Supplementary material in ancillary files

We report on the heteroepitaxial stabilization of YCrO3 ultra-thin films on LSAT (001) substrate. Using a combination of resonant X-ray absorption spectroscopy (XAS) and atomic multiplet cluster calculation, the electronic structure of YCrO3 thin film was investigated. Polarization dependent Cr L3,2 edge XAS measurement reveal the presence of an anomalous orbital polarization uncharacteristic of a 3d3 electronic system. Atomic multiplet calculations demonstrate the critical importance of charge transfer energy, Coulomb correlation strength and hopping interaction in stabilizing this unusual orbital polarized state likely connected to the bulk multiferroicity.

Understanding, creating, and manipulating spin polarization of two-dimensional electron gases at complex oxide interfaces presents an experimental challenge. For example, despite almost a decade long research effort, the microscopic origin of ferromagnetism in LaAlO3/SrTiO3 heterojunction is still an open question. Here, by using a prototypical two-dimensional electron gas (2DEG) which emerges at the interface between band insulator SrTiO3 and antiferromagnetic Mott insulator LaTiO3 , the experiment reveals the evidence for magnetic phase separation in hole-doped Ti d1 t2g system resulting in spin-polarized 2DEG. The details of electronic and magnetic properties of the 2DEG were investigated by temperature-dependent d.c. transport, angle-dependent X-ray photoemission spectroscopy, and temperature-dependent magnetoresistance. The observation of clear hysteresis in magnetotransport at low magnetic fields implies spin-polarization from magnetic islands in the hole rich LaTiO3 near the interface. These findings emphasize the role of magnetic instabilities in doped Mott insulators thus providing another path for designing all-oxide structures relevant to spintronics applications.

Transition metal oxides (TMOs) are complex electronic systems which 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 we report the discovery of a memory effect in both systems, manifest 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, we find 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 critical 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., Comment: 18 pages, 4 figures, supporting information in publisher web-site

The perovksite rare-earth nickelates, RNiO$_3$ (R=La ... Lu), are a class of materials displaying a rich phase-diagram of metallic and insulating phases associated with charge and magnetic order. Being in the charge transfer regime, Ni$^{3+}$ in octahedral coordination displays a strong hybridization with oxygen to form $3d$ - $2p$ mixed states, which results in a strong admixture of $3d^8\underline{L}$ into $3d^7$, where $\underline{L}$ denotes a hole on the oxygen. To understand the nature of this strongly hybridized ground state, we present a detailed study of the Ni and O electronic structure using high-resolution soft X-ray Absorption Spectroscopy (XAS). Through a comparison of the evolution of the XAS line-shape at Ni L- and O K-edges across the phase diagram, we explore the changes in the electronic signatures in connection with the insulating and metallic phases that support the idea of hybridization playing a fundamental role., Comment: 7 pages, 6 figures, Submitted to Journal of Electron Spectroscopy and Related Phenomena

Finding new collective electronic states in materials is one of the fundamental goals of condensed matter physics. Atomic-scale superlattices formed from transition metal oxides are a particularly appealing hunting ground for new physics. In bulk form, transition metal oxides exhibit a remarkable range of magnetic, superconducting, and multiferroic phases that are of great scientific interest and are potentially capable of providing innovative energy, security, electronics and medical technology platforms. In superlattices new states may emerge at the interfaces where dissimilar materials meet. Here we illustrate the essential features that make transition metal oxide-based heterostructures an appealing discovery platform for emergent properties with a few selected examples, showing how charge redistributes, magnetism and orbital polarization arises and ferroelectric order emerges from heterostructures comprised of oxide components with nominally contradictory behavior with the aim providing insight into the creation and control of novel behavior at oxide interfaces by suitable mechanical, electrical or optical boundary conditions and excitations., Comment: 16 pages, 5 figures

Ultrafast pump-probe spectroscopy is a powerful tool to study the nonequilibrium dynamics in high-Tc cuprate superconductors. The photo-induced quasiparticle (QP) dynamics revealed by pump-probe spectroscopy are sensitive to the near-Fermi level electronic structures. Here we review several selected examples to illustrate the enduring challenges including pairing glue, phase separation, and phase transitions in cuprate superconductors. We also present the data obtained on thin films of YBa2Cu3O7-{\delta} in connection to these issues., Comment: Invited paper for "current perspectives" in Journal of Magnetism and Magentic Materials

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 N\'eel 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., Comment: For updated published version see the link below