Interfacial Electron-Phonon Coupling Constants Extracted from Intrinsic Replica Bands in Monolayer FeSe/SrTiO_{3}.

The observation of replica bands by angle-resolved photoemission spectroscopy has ignited interest in the study of electron-phonon coupling at low carrier densities, particularly in monolayer FeSe/SrTiO_{3}, where the appearance of replica bands has motivated theoretical work suggesting that the interfacial coupling of electrons in the FeSe layer to optical phonons in the SrTiO_{3} substrate might contribute to the enhanced superconducting pairing temperature. Alternatively, it has also been recently proposed that such replica bands might instead originate from extrinsic final state losses associated with the photoemission process. Here, we perform a quantitative examination of replica bands in monolayer FeSe/SrTiO_{3}, where we are able to conclusively demonstrate that the replica bands are indeed signatures of intrinsic electron-boson coupling, and not associated with final state effects. A detailed analysis of the energy splittings and relative peak intensities between the higher-order replicas, as well as other self-energy effects, allows us to determine that the interfacial electron-phonon coupling in the system corresponds to a value of λ=0.19±0.02, providing valuable insights into the enhancement of superconductivity in monolayer FeSe/SrTiO_{3}. The methodology employed here can also serve as a new and general approach for making more rigorous and quantitative comparisons to theoretical calculations of electron-phonon interactions and coupling constants.

Measurements of Oxygen Electroadsorption Energies and Oxygen Evolution Reaction on RuO2(110): A Discussion of the Sabatier Principle and Its Role in Electrocatalysis.

We report the hydroxide (OHad) and oxide (Oad) experimental electroadsorption free energies, their dependences on pH, and their correlations to the oxygen evolution reaction (OER) electrocatalysis on RuO2(110) surface. The Sabatier principle predicts that catalyst is most active when the intermediate stabilization is moderate, not too strong such that the bound intermediate disrupts the subsequent catalytic cycle, nor too weak such that the surface is ineffective. For decades, researchers have used this concept to rationalize the activity trend of many OER electrocatalysts including RuO2, which is among the state-of-the-art OER catalysts. In this article, we report an experimental assessment of the Sabatier principle by comparing the oxygen electroadsorption energy to the OER electrocatalysis for the first time on RuO2. We find that the OHad and Oad electroadsorption energies on RuO2(110) depend on pH and obey the scaling relation. However, we did not observe a direct correlation between the OHad and Oad electroadsorption energies and the OER activity in the comparative analysis that includes both RuO2(110) and IrO2(110). Our result raises a question of whether the Sabatier principle can describe highly active electrocatalysts, where the kinetic aspects may influence the electrocatalysis more strongly than the electroadsorption energy, which captures only the thermodynamics of the intermediates and not yet kinetics.

Interfacial charge transfer and persistent metallicity of ultrathin SrIrO3/SrRuO3 heterostructures.

Interface quantum materials have yielded a plethora of previously unknown phenomena, including unconventional superconductivity, topological phases, and possible Majorana fermions. Typically, such states are detected at the interface between two insulating constituents by electrical transport, but whether either material is conducting, transport techniques become insensitive to interfacial properties. To overcome these limitations, we use angle-resolved photoemission spectroscopy and molecular beam epitaxy to reveal the electronic structure, charge transfer, doping profile, and carrier effective masses in a layer-by-layer fashion for the interface between the Dirac nodal-line semimetal SrIrO3 and the correlated metallic Weyl ferromagnet SrRuO3. We find that electrons are transferred from the SrIrO3 to SrRuO3, with an estimated screening length of λ = 3.2 ± 0.1 Å. In addition, we find that metallicity is preserved even down to a single SrIrO3 layer, where the dimensionality-driven metal-insulator transition typically observed in SrIrO3 is avoided because of strong hybridization of the Ir and Ru t2g states.

Strong interlayer interactions in bilayer and trilayer moiré superlattices.

Moiré superlattices constructed from transition metal dichalcogenides have demonstrated a series of emergent phenomena, including moiré excitons, flat bands, and correlated insulating states. All of these phenomena depend crucially on the presence of strong moiré potentials, yet the properties of these moiré potentials, and the mechanisms by which they can be generated, remain largely open questions. Here, we use angle-resolved photoemission spectroscopy with submicron spatial resolution to investigate an aligned WS2/WSe2 moiré superlattice and graphene/WS2/WSe2 trilayer heterostructure. Our experiments reveal that the hybridization between moiré bands in WS2/WSe2 exhibits an unusually large momentum dependence, with the splitting between moiré bands at the Γ point more than an order of magnitude larger than that at K point. In addition, we discover that the same WS2/WSe2 superlattice can imprint an unexpectedly large moiré potential on a third, separate layer of graphene (g/WS2/WSe2), suggesting new avenues for engineering two-dimensional moiré superlattices.

Realization of Epitaxial Thin Films of the Topological Crystalline Insulator Sr3 SnO.

Topological materials are derived from the interplay between symmetry and topology. Advances in topological band theories have led to the prediction that the antiperovskite oxide Sr3 SnO is a topological crystalline insulator, a new electronic phase of matter where the conductivity in its (001) crystallographic planes is protected by crystallographic point group symmetries. Realization of this material, however, is challenging. Guided by thermodynamic calculations, a deposition approach is designed and implemented to achieve the adsorption-controlled growth of epitaxial Sr3 SnO single-crystal films by molecular-beam epitaxy (MBE). In situ transport and angle-resolved photoemission spectroscopy measurements reveal the metallic and electronic structure of the as-grown samples. Compared with conventional MBE, the used synthesis route results in superior sample quality and is readily adapted to other topological systems with antiperovskite structures. The successful realization of thin films of Sr3 SnO opens opportunities to manipulate topological states by tuning symmetries via strain engineering and heterostructuring.