Influence of Heterointerfaces on the Kinetics of Oxygen Surface Exchange on Epitaxial La1.85Sr0.15CuO4 Thin Films

Considerable attention has been directed to understanding the influence of heterointerfaces between Ruddlesden-Popper (RP) phases and ABO(3) perovskites on the kinetics of oxygen electrocatalysis at elevated temperatures. Here, we report the effect of heterointerfaces on the oxygen surface exchange kinetics by employing heteroepitaxial oxide thin films formed by decorating LaNiO3 (LNO) on La1.85Sr0.15CuO4 (LSCO) thin films. Regardless of LNO decoration, tensile in-plane strain on LSCO films does not change. The oxygen surface exchange coefficients (k(chem)) of LSCO films extracted from electrical conductivity relaxation curves significantly increase with partial decorations of LNO, whereas full LNO coverage leads to the reduction in the k(chem) of LSCO films. The activation energy for oxygen exchange in LSCO films significantly decreases with partial LNO decorations in contrast with the full coverage of LNO. Optical spectroscopy reveals the increased oxygen vacancies in the partially covered LSCO films relative to the undecorated LSCO film. We attribute the enhanced oxygen surface exchange kinetics of LSCO to the increased oxygen vacancies by creating the heterointerface between LSCO and LNO

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

Hund's rule coupling ($\textit{J}$) 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, $\textit{J}$ 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 $\textit{J}$ related phenomena without inducing inhomogeneities. By growing SrRuO$_3$ monolayers on various substrates with symmetry-preserving interlayers, we gradually tune the crystal field splitting and thus the orbital degeneracy of the Ru \textit{t_2_g$}$ 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 $\textit{d$_x_y} band and a Mott gap in the \textit{d_x$$_z$$_/$$_y$$_z} bands. Our study provides an effective experimental method for investigation of orbital-selective phenomena in multi-orbital materials

Electronic Structure and Insulating Gap in Epitaxial VO\u3csub\u3e2\u3c/sub\u3e Polymorphs

Determining the origin of the insulating gap in the monoclinic VO2(M1) is a long-standing issue. The difficulty of this study arises from the simultaneous occurrence of structural and electronic transitions upon thermal cycling. Here, we compare the electronic structure of the M1 phase with that of single crystalline insulating VO2(A) and VO2(B) thin films to better understand the insulating phase of VO2. As these A and B phases do not undergo a structural transition upon thermal cycling, we comparatively study the origin of the gap opening in the insulating VO2 phases. By x-ray absorption and optical spectroscopy, we find that the shift of unoccupied t2g orbitals away from the Fermi level is a common feature, which plays an important role for the insulating behavior in VO2 polymorphs. The distinct splitting of the half-filled t2g orbital is observed only in the M1 phase, widening the bandgap up to ∼0.6 eV. Our approach of comparing all three insulating VO2 phases provides insight into a better understanding of the electronic structure and the origin of the insulating gap in VO2

Strong spin-phonon coupling unveiled by coherent phonon oscillations in Ca2RuO4

© 2019 American Physical Society. We utilize near-infrared femtosecond pulses to investigate coherent phonon oscillations of Ca2RuO4. The coherent Ag phonon mode of the lowest frequency changes abruptly not only its amplitude but also the oscillation phase as the spin order develops. In addition, the phonon mode shows a redshift entering the magnetically ordered state, which indicates a spin-phonon coupling in the system. Density functional theory calculations reveal that the Ag oscillations result in octahedral tilting distortions, which are exactly in sync with the lattice deformation driven by the magnetic ordering. We suggest that the structural distortions by the spin-phonon coupling can induce the unusual oscillation phase shift between impulsive and displacive type oscillation

Honeycomb oxide heterostructure: a new platform for Kitaev quantum spin liquid

Kitaev quantum spin liquid, massively quantum entangled states, is so scarce in nature that searching for new candidate systems remains a great challenge. Honeycomb heterostructure could be a promising route to realize and utilize such an exotic quantum phase by providing additional controllability of Hamiltonian and device compatibility, respectively. Here, we provide epitaxial honeycomb oxide thin film Na3Co2SbO6, a candidate of Kitaev quantum spin liquid proposed recently. We found a spin glass and antiferromagnetic ground states depending on Na stoichiometry, signifying not only the importance of Na vacancy control but also strong frustration in Na3Co2SbO6. Despite its classical ground state, the field-dependent magnetic susceptibility shows remarkable scaling collapse with a single critical exponent, which can be interpreted as evidence of quantum criticality. Its electronic ground state and derived spin Hamiltonian from spectroscopies are consistent with the predicted Kitaev model. Our work provides a unique route to the realization and utilization of Kitaev quantum spin liquid

Orbital-selective Mott and Peierls transition in HxVO2

Materials displaying metal-insulator transitions (MITs) as a function of external parameters such as temperature, pressure, or composition are most intriguing from the fundamental point of view and also hold high promise for applications. Vanadium dioxide (VO2) is one of the most prominent examples of MIT having prospective applications ranging from intelligent coatings, infrared sensing, or imaging, to Mott memory and neuromorphic devices. The key aspects conditioning possible applications are the controllability and reversibility of the transition. Here we present an intriguing MIT in hydrogenated vanadium dioxide, HxVO2. The transition relies on an increase of the electron occupancy through hydrogenation on the transition metal vanadium, driving the system insulating by a hybrid of two distinct MIT mechanisms. The insulating phase observed in HVO2 with a nominal d2 electronic configuration contrasts with other rutile d2 systems, most of which are metallic. Using spectroscopic tools and state-of-the-art many-body electronic structure calculations, our investigation reveals a correlation-enhanced Peierls and a Mott transition taking place in an orbital-selective manner cooperate to stabilize an insulating phase. The identification of the hybrid mechanism for MIT controlled by hydrogenation opens the way to radically design strategies for future correlated oxide devices by controlling phase reversibly while maintaining high crystallinity

High sensitivity bolometers based on metal nanoantenna dimers with a nanogap filled with vanadium dioxide

One critical factor for bolometer sensitivity is efficient electromagnetic heating of thermistor materials, which plasmonic nanogap structures can provide through the electric field enhancement. In this report, using finite element method simulation, electromagnetic heating of nanorod dimer antennas with a nanogap filled with vanadium dioxide (VO2) was studied for long-wavelength infrared detection. Because VO2 is a thermistor material, the electrical resistance between the two dimer ends depends on the dimer's temperature. The simulation results show that, due to the high heating ability of the nanogap, the temperature rise is several times higher than expected from the areal coverage. This excellent performance is observed over various nanorod lengths and gap widths, ensuring wavelength tunability and ultrafast operating speed, thereby making the dimer structures a promising candidate for high sensitivity bolometers

Preparation of large Cu3Sn single crystal by Czochralski method

Cu3Sn was recently predicted to host topological Dirac fermions, but related research is still in its infancy. The growth of large and high-quality Cu3Sn single crystals is, therefore, highly desired to investigate the possible topological properties. In this work, we report the single crystal growth of Cu3Sn by Czochralski (CZ) method. Crystal structure, chemical composition, and transport properties of Cu3Sn single crystals were analyzed to verify the crystal quality. Notably, compared to the mm-sized crystals from a molten Sn flux, the cm-sized crystals obtained by the CZ method are free from contamination from flux materials, paving the way for the follow-up works