Current silicon-based CMOS devices face physical limitations in downscaling size and power loss, restricting their capability to meet the demands for data storage and information processing of emerging technologies. One possible alternative is to encode the information in a non-volatile magnetic state and manipulate this spin state electronically, as in spintronics. However, current spintronic devices rely on the current-driven control of magnetization, which involves Joule heating and power dissipation. This limitation has motivated intense research into the voltage-driven manipulation of spin signals to achieve energy-efficient device operation. Here, we show non-volatile control of spin-charge conversion at room temperature in graphene-based heterostructures through Fermi level tuning. We use a polymeric ferroelectric film to induce non-volatile charging in graphene. To demonstrate the switching of spin-to-charge conversion we perform ferromagnetic resonance and inverse Edelstein effect experiments. The sign change of output voltage is derived by the change of carrier type, which can be achieved solely by a voltage pulse. Our results provide an alternative approach for the electric-field control of spin-charge conversion, which constitutes a building block for the next generation of spin-orbitronic memory and logic devices.

Transparent conducting oxides are crucial in the field of optoelectronics, and SrNbO3 has emerged as a promising candidate because it can outperform commonly used indium tin oxides due to its novel functionality. However, experimental investigations of SrNbO3 are challenging because it undergoes topotactic phase transition to exhibit insulating behavior. Here, we investigate the pivotal role of SrNbO3 stoichiometry to enhance its performance as a transparent conducting oxide. Results indicate the optoelectronic properties of SrNbO3 are highly dependent on its intrinsic lattice parameters and stoichiometry. Films with lattice parameters close to those of pure SrNbO3 exhibit excellent conductivity and transmittance in the visible range, while off-stoichiometry diminishes optoelectronic properties. Our stoichiometric sample demonstrates a record-high figure of merit for SrNbO3, considerably surpassing that of indium tin oxide by an order of magnitude. Thus, this study paves the way for production of high-quality SrNbO3 and leveraging its novel functionalities in optoelectronic applications.

Identifying the magnetic state of materials is of great interest in a wide range of applications, but direct identification is not always straightforward due to limitations in neutron scattering experiments. In this work, we present a machine-learning approach using decision-tree algorithms to identify magnetism from the spin-integrated excitation spectrum, such as the density of states. The dataset was generated by Hartree-Fock mean-field calculations of candidate antiferromagnetic orders on a Wannier Hamiltonian, extracted from first-principle calculations targeting \boo. Our machine learning model was trained using various types of spectral data, including local density of states, momentum-resolved density of states at high-symmetry points, and the lowest excitation energies from the Fermi level. Although the density of states shows good performance for machine learning, the broadening method had a significant impact on the model’s performance. We improved the model’s performance by designing the excitation energy as a feature for machine learning, resulting in excellent classification of antiferromagnetic order, even for test samples generated by different methods from the training samples used for machine learning.

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.

The oxide interfaces between materials with different structural symmetries have been actively studied due to their novel physical properties. However, the investigation of intriguing interfacial phenomena caused by the oxygen octahedral tilt (OOT) proximity effect has not been fully exploited, as there is still no clear understanding of what determines the proximity length and what the underlying control mechanism is. Here, we achieved scalability of the OOT proximity effect in SrRuO₃ (SRO) by epitaxial strain near the SRO/SrTiO3 heterointerface. We demonstrated that the OOT proximity length scale of SRO is extended from 4 unit cells to 14 unit cells by employing advanced scanning transmission electron microscopy. We also suggest that this variation may originate from changes in phonon dispersions due to electron–phonon coupling in SRO. This study will provide in-depth insights into the structural gradients of correlated systems and facilitate potential device applications.

The oxide interfaces between materials with different structural symmetries have been actively studied due to their novel physical properties. However, the investigation of intriguing interfacial phenomena caused by the oxygen octahedral tilt (OOT) proximity effect has not been fully exploited, as there is still no clear understanding of what determines the proximity length and what the underlying control mechanism is. Here, we achieved scalability of the OOT proximity effect in SrRuO3 (SRO) by epitaxial strain near the SRO/SrTiO3 heterointerface. We demonstrated that the OOT proximity length scale of SRO is extended from 4 unit cells to 14 unit cells by employing advanced scanning transmission electron microscopy. We also suggest that this variation may originate from changes in phonon dispersions due to electron–phonon coupling in SRO. This study will provide in-depth insights into the structural gradients of correlated systems and facilitate potential device applications.

The heavy fermion state with Kondo-hybridisation (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localised electrons appropriate for Kondo pairing. Here, we report a substitution- and temperature-dependent angle-resolved photoemission study on 4d Ca_2−xSr_xRuO₄, which shows the signature of KH. We observed a spectral weight transfer in the γ-band, reminiscent of an orbital-selective Mott phase (OSMP). The Mott localised γ-band induces the KH with an itinerant β-band, resulting in spectral weight suppression around the Fermi level. Our work demonstrates the evolution of the OSMP with possible KH among 4d electrons, and thereby expands the material boundary of Kondo physics to 4d multi-orbital systems.

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 Y₂Ir₂O₇ 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 Y₂Ir₂O₇ 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.

Correlated electrons in transition metal oxides exhibit a variety of emergent phases. When transition metal oxides are confined to a single-atomic-layer thickness, experiments so far have shown that they usually lose diverse properties and become insulators. In an attempt to extend the range of electronic phases of the single-atomic-layer oxide, we search for a metallic phase in a monolayer-thick epitaxial SrRuO₃ film. Combining atomic-scale epitaxy and angle-resolved photoemission measurements, we show that the monolayer SrRuO₃ is a strongly correlated metal. Systematic investigation reveals that the interplay between dimensionality and electronic correlation makes the monolayer SrRuO₃ an incoherent metal with orbital-selective correlation. Furthermore, the unique electronic phase of the monolayer SrRuO₃ is found to be highly tunable, as charge modulation demonstrates an incoherent-to-coherent crossover of the two-dimensional metal. Our work emphasizes the potentially rich phases of single-atomic-layer oxides and provides a guide to the manipulation of their two-dimensional correlated electron systems.

A van Hove singularity (VHS) often significantly amplifies the electronic instability of a crystalline solid, including correlation-induced phenomena such as Hund’s metallicity. We perform a systematic study on the interplay between Hund’s coupling and electronic structures with a VHS focusing on Hund’s metallicity. We construct a simplified tight-binding model targeting cubic perovskite materials and test the effects of the VHS utilizing dynamical mean-field theory with an exact diagonalization solver. The quasiparticle weight and the low-frequency power exponent of the self-energy provide a quantitative estimation of metallicity over the phase diagram. We find the VHS to substantially enhance Hund’s metallicity. The results here suggest a range of parameters through which a VHS can bring great synergy with Hund’s coupling.

The spin-orbit entangled (SOE) J_eff state has been a fertile ground to study quantum phenomena. Contrary to the conventional weakly correlated J_eff=1/2 state of 4d and 5d transition metal compounds, the ground state of CuAl₂O₄ hosts a J_eff=1/2 state with a strong correlation of Coulomb U. Here, we report that, surprisingly, Cu²⁺ ions of CuAl₂O₄ overcome the otherwise usually strong Jahn-Teller distortion and instead stabilize the SOE state, although the cuprate has relatively small spin-orbit coupling. From the x-ray absorption spectroscopy and high-pressure x-ray diffraction studies, we obtained definite evidence of the J_eff=1/2 state with a cubic lattice at ambient pressure. We also found the pressure-induced structural transition to a compressed tetragonal lattice consisting of the spin-only S=1/2 state for pressure P_c>8GPa. This phase transition from the Mott insulating J_eff=1/2 to the S=1/2states is a unique phenomenon. Our study offers an example of the SOE Jeff state under strong electron correlation and its pressure-induced transition to the S=1/2 state.

Rotation of MO6 (M = transition metal) octahedra is a key determinant of the physical properties of perovskite materials. Therefore, tuning physical properties, one of the most important goals in condensed matter research, may be accomplished by controlling octahedral rotation (OR). In this study, it is demonstrated that OR can be driven by an electric field in Sr₂RuO₄. Rotated octahedra in the surface layer of Sr₂RuO₄ are restored to the unrotated bulk structure upon dosing the surface with K. Theoretical investigation shows that OR in Sr₂RuO₄ originates from the surface electric field, which can be tuned via the screening effect of the overlaid K layer. This work establishes not only that variation in the OR angle can be induced by an electric field, but also provides a way to control OR, which is an important step toward in situ control of the physical properties of perovskite oxides.

We investigate the roles of spin-orbit coupling and the Van Hove singularity in the dynamical properties of Sr₂RuO₄, which become prominent at zero and very low temperature, by means of density functional theory plus dynamical mean-field theory with an exact diagonalization solver. We examine the crossover between a Fermi liquid and a Hund's metal for a wide range of temperatures and Hund's coupling. In the absence of doping, we confirm that the Fermi liquid persists at zero temperature even with nonzero Hund's coupling. The freezing-moment mechanism suggests that thermal fluctuations lead to a suppression of the Fermi liquid phase and promote Hund's metallicity with incoherence. We show that the Van Hove singularity is an additional key ingredient to drive the suppression at very low temperature by observing a doping dependence of the freezing or long-lived paramagnetic moments. The role of spin-orbit coupling is marked by an amplified Van Vleck contribution of spin susceptibility, significantly promoting Hund's metallicity. Together with the known doping dependence of Hund's metallicity, the additional Van Hove singularity doping dependence found here may allow for the control of the Hund's metallicity of Sr₂RuO₄(t⁴_2g) by a fine tuning of the doping or possibly even strain.

Using first-principles calculations, we show that topological quantum phase transitions are driven by external electric fields in thin films of Sb₂Te₃. The film, as the applied electric field normal to its surface increases, is transformed from a normal insulator to a topological insulator or vice versa depending on the film thickness. We identify the band topology by directly calculating the invariant from electronic wave functions. The dispersion of edge states is also found to be consistent with the bulk band topology in view of the bulk-boundary correspondence. We present possible applications of the topological phase transition as an on/off switch of the topologically protected edge states in nano-scale devices.

We propose that the existence of local orbital angular momentum (OAM) on the surfaces of high-Z materials plays a crucial role in the formation of Rashba-type surface band splitting. Local OAM state in a Bloch wave function produces an asymmetric charge distribution (electric dipole). The surface-normal electric field then aligns the electric dipole and results in chiral OAM states and the relevant Rashba-type splitting. Therefore, the band splitting originates from electric dipole interaction, not from the relativistic Zeeman splitting as proposed in the original Rashba picture. The characteristic spin chiral structure of Rashba states is formed through the spin-orbit coupling and thus is a secondary effect to the chiral OAM. Results from first-principles calculations on a single Bi layer under an external electric field verify the key predictions of the new model.

We have investigated the electronic structure of double perovskites, Ba₂FeReO₆ (metallic) and Ca₂FeReO₆ (insulating) using optical and x-ray absorption spectroscopy. By comparing the experimental results with the density functional theory calculations, we found that the electronic structure of Ba₂FeReO₆ could be determined from the interaction of the electron correlation and spin–orbit coupling. On the other hand, for Ca₂FeReO₆, the lattice distortion and electron correlation are important in determining the electronic structure. Additionally, the insulating gap in Ca₂FeReO₆ is realized by the spin–orbit coupling. Our work shows that the subtle interplay of the spin–orbit interaction, electron correlation, and lattice distortion should be taken into account to understand the electronic structure of the 5d transition metal oxides.

We report on a fundamental thickness limit of the itinerant ferromagnetic oxide SrRuO₃ that might arise from the orbital-selective quantum confinement effects. Experimentally, SrRuO₃ films remain metallic even for a thickness of 2 unit cells (uc), but the Curie temperature T_C starts to decrease at 4 uc and becomes zero at 2 uc. Using the Stoner model, we attributed the T_CC decrease to a decrease in the density of states (N_o). Namely, in the thin film geometry, the hybridized Ru d_yz,zx orbitals are terminated by top and bottom interfaces, resulting in quantum confinement and reduction of N_o.

We present an extension of the local moment approach to the Anderson impurity model with spin-dependent hybridization. By employing the two-self-energy description, as originally proposed by Logan and co-workers, we applied the symmetry restoration condition for the case with spin-dependent hybridization. Self-consistent ground states were determined through variational minimization of the ground state energy. The results obtained with our spin-dependent local moment approach applied to a quantum dot system coupled to ferromagnetic leads are in good agreement with those obtained from previous work using numerical renormalization group calculations.

The infinite-U Anderson model coupled to a Jahn-Teller phonon is studied using the slave boson method on the basis of the large degeneracy expansion (1∕N) scheme. The model Hamiltonian acts on the orbital degrees of freedom. The main focus is on the interplay between strong local electron correlation and weak Jahn-Teller electron-phonon interaction. The Kondo temperature is found to decrease by Jahn-Teller interaction. The influence of the Jahn-Teller interaction on dynamical correlation functions is very significant, in sharp contrast with the case of the Holstein-type phonon which couples to charge degrees of freedom.