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Register a new userProbing single unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission
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Control of structural couplings at the complex-oxide interfaces is a powerful platform for creating new ultrathin layers with electronic and magnetic properties unattainable in the bulk. However, with the capability to design and control the electronic structure of such buried layers and interfaces at a unit-cell level, a new challenge emerges to be able to probe these engineered emergent phenomena with depth-dependent atomic resolution as well as element- and orbital selectivity. Here, we utilize a combination of core-level and valence-band soft x-ray standing-wave photoemission spectroscopy, in conjunction with scanning transmission electron microscopy, to probe the depth-dependent and single-unit-cell resolved electronic structure of an isovalent manganite superlattice [Eu0.7Sr0.3MnO3/La0.7Sr0.3MnO3]x15 wherein the electronic-structural properties are intentionally modulated with depth via engineered oxygen octahedra rotations/tilts and A-site displacements. Our unit-cell resolved measurements reveal significant transformations in the local chemical and electronic valence-band states, which are consistent with the layer-resolved first-principles theoretical calculations, thus opening the door for future depth-resolved studies of a wide variety of hetero-engineered material systems.
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When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO2, which consists of alternating layers of metallic Pd and Mott-insulating CoO2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO2, we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured valence band spectrum into contributions from Pd and CoO2 layers. Computationally, we find that many-body interactions in Pd and CoO2 layers are highly different. Holes in the CoO2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials.
Continuing the photoemission study begun with the work of Opeil et al. [Phys. Rev. B textbf{73}, 165109 (2006)], in this paper we report results of an angle-resolved photoemission spectroscopy (ARPES) study performed on a high-quality single-crystal $alpha$-uranium at 173 K. The absence of surface-reconstruction effects is verified using X-ray Laue and low-energy electron diffraction (LEED) patterns. We compare the ARPES intensity map with first-principles band structure calculations using a generalized gradient approximation (GGA) and we find good correlations with the calculated dispersion of the electronic bands.
Interface can be a fertile ground for exotic quantum states, including topological superconductivity, Majorana mode, fractal quantum Hall effect, unconventional superconductivity, Mott insulator, etc. Here we grow single-unit-cell (1UC) FeTe film on NbSe2 single crystal by molecular beam epitaxy (MBE) and investigate the film in-situ with home-made cryogenic scanning tunneling microscopy (STM) and non-contact atomic force microscopy (AFM) combined system. We find different stripe-like superlattice modulations on grown FeTe film with different misorientation angles with respect to NbSe2 substrate. We show that these stripe-like superlattice modulations can be understood as moire pattern forming between FeTe film and NbSe2 substrate. Our results indicate that the interface between FeTe and NbSe2 is atomically sharp. By STM-AFM combined measurement, we suggest the moire superlattice modulations have an electronic origin when the misorientation angle is relatively small (<= 3 degree) and have structural relaxation when the misorientation angle is relatively large (>= 10 degree).
Inversion symmetry breaking is a ubiquitous concept in condensed-matter science. On the one hand, it is a prerequisite for many technologically relevant effects such as piezoelectricity, photovoltaic and nonlinear optical properties and spin-transport phenomena. On the other hand, it may determine abstract properties such as the electronic topology in quantum materials. Therefore, the creation of materials where inversion symmetry can be turned on or off by design may be the ultimate route towards controlling parity-related phenomena and functionalities. Here, we engineer the symmetry of ultrathin epitaxial oxide films by sub-unit-cell growth control. We reversibly activate and deactivate inversion symmetry in the layered hexagonal manganites, h-RMnO$_3$ with R = Y, Er, Tb. While an odd number of half-unit-cell layers exhibits a breaking of inversion symmetry through its arrangement of MnO$_5$ bipyramids, an even number of such half-unit-cell layers takes on a centrosymmetric structure. Here we control the resulting symmetry by tracking the growth in situ via optical second-harmonic generation. We furthermore demonstrate that our symmetry engineering works independent of the choice of R and even in heterostructures mixing constituents with different R in a two-dimensional growth mode. Symmetry engineering on the atomic level thus suggests a new platform for the controlled activation and deactivation of symmetry-governed functionalities in oxide-electronic epitaxial thin films.
Electronic structure of single crystalline Ba(Zn$_{0.875}$Mn$_{0.125}$)$_{2}$As$_{2}$, parent compound of the recently founded high-temperature ferromagnetic semiconductor, was studied by high-resolution photoemission spectroscopy (ARPES). Through systematically photon energy and polarization dependent measurements, the energy bands along the out-of-plane and in-plane directions were experimentally determined. Except the localized states of Mn, the measured band dispersions agree very well with the first-principle calculations of undoped BaZn$_{2}$As$_{2}$. A new feature related to Mn 3d states was identified at the binding energies of about -1.6 eV besides the previously observed feature at about -3.3 eV. We suggest that the hybridization between Mn and As orbitals strongly enhanced the density of states around -1.6 eV. Although our resolution is much better compared with previous soft X-ray photoemission experiments, no clear hybridization gap between Mn 3d states and the valence bands proposed by previous model calculations was detected.
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