Michael Schneider

Innovative approaches to study buried interfaces and heterogeneous interactions under reaction conditions are crucial for advancing energy and catalytic materials. Our near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) setup is equipped with a tricolor x-ray source, with Al Kα, Ag Lα, and Cr Kα excitation energies, enabling information depth–selective operando and in situ analysis of solid-liquid, solid-gas, and solid-solid interfaces. We present three case studies to demonstrate the systems’ capabilities. First, we compare experimental depth profiling of a LaMnO ₃ /LaFeO ₃ /Nb:SrTiO ₃ multilayer with SESSA (simulation of electron spectra for surface analysis) simulations. Second, we examine the oxidation and reduction of Fe _x O _y as a function of environment and temperature. Last, the Pt/liquid electrolyte interface is examined, revealing surface oxidation in the absence of bulk oxidation. As our results confirm, the unique combination of a NAP-XPS with the tricolor x-ray source empowers laboratory-based in situ and operando XPS characterization of advanced materials under reaction conditions in a wide range of applications.

Quantum materials are notoriously sensitive to their environments, where small perturbations can tip a system toward one of several competing ground states. Graphene hosts a rich assortment of such competing phases, including a bond density wave instability (“Kekulé distortion”) that couples electrons at the K/K′ valleys and breaks the lattice symmetry. Here, we report observations of a ubiquitous Kekulé distortion across multiple graphene systems. We show that extremely dilute concentrations of surface atoms (less than three adsorbed atoms every 1000 graphene unit cells) can self-assemble and trigger the onset of a global Kekulé density wave phase. Combining complementary momentum-sensitive angle-resolved photoemission spectroscopy (ARPES) and low-energy electron diffraction (LEED) measurements, we confirm the presence of this density wave phase and observe the opening of an energy gap. Our results reveal an unexpected sensitivity of the graphene lattice to dilute surface disorder and show that adsorbed atoms offer an attractive route toward designing novel phases in two-dimensional materials.

Among the iron-based superconductors, LiFeAs is unrivaled in the simplicity of its crystal structure and phase diagram. However, our understanding of this canonical compound suffers from conflict between mutually incompatible descriptions of the material's electronic structure, as derived from contradictory interpretations of the photoemission record. Here we explore the challenge of interpretation in such experiments. By combining comprehensive photon energy- and polarization-dependent angle-resolved photoemission spectroscopy (ARPES) measurements with numerical simulations, we establish the providence of several contradictions in the present understanding of this and related materials. We identify a confluence of surface-related issues which have precluded unambiguous identification of both the number and the dimensionality of the Fermi-surface sheets. Ultimately, we arrive at a scenario which supports indications of topologically nontrivial states while also being incompatible with superconductivity as a spin-fluctuation-driven Fermi-surface instability.

The mechanism of the enhanced superconductivity in monolayer FeSe/SrTiO₃ has been enthusiastically studied and debated over the past decade. One specific observation has been taken to be of central importance: the replica bands in the photoemission spectrum. Although suggestive of electron-phonon interaction in the material, the essence of these spectroscopic features remains highly controversial. In this work, we conduct angle-resolved photoemission spectroscopy measurements on monolayer FeSe/SrTiO₃ using linearly polarized photons. This configuration enables unambiguous characterization of the valence electronic structure with a suppression of the spectral background. We consistently observe high-order replica bands derived from various Fe 3d bands, similar to those observed on bare SrTiO₃. The intensity of the replica bands is unexpectedly high and different between d_xy and d_yz bands. Our results provide new insights on the electronic structure of this high-temperature superconductor and the physical origin of the photoemission replica bands.

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) provides access to the ultrafast evolution of electrons and many-body interactions in solid-state systems. However, the momentum- and energy-resolved transient photoemission intensity may not be unambiguously described by the intrinsic relaxation dynamics of photoexcited electrons alone. The interpretation of the time-dependent photoemission signal can be affected by the transient evolution of the electronic distribution, and both the one-electron removal spectral function as well as the photoemission matrix elements. Here we investigate the topological insulator Bi_1.1Sb_0.9Te₂S to demonstrate, by means of a detailed probe-polarization dependent study, the transient contribution of matrix elements to TR-ARPES.

Complex electron interactions underlie the electronic structure of several families of quantum materials. In particular, the strong electron Coulomb repulsion is considered the key ingredient to describing the emergence of exotic and/or ordered phases of quantum matter, from high-temperature superconductivity to charge- and magnetic-order. However, a comprehensive understanding of fundamental electronic properties of quantum materials is often complicated by the appearance of an enigmatic partial suppression of low-energy electronic states, known as the pseudogap. Here we take advantage of ultrafast angle-resolved photoemission spectroscopy to unveil the temperature evolution of the low-energy density of states in the electron-doped cuprate Nd_2-xCe_xCuO₄, an emblematic system where the pseudogap intertwines with magnetic degrees of freedom. Using an optical excitation we drive the electronic system across the pseudogap onset temperature T*, and we report the direct relation between the momentum-resolved pseudogap spectral features and the spin-correlation length with a remarkable sensitivity. This transient approach, corroborated by mean-field model calculations, allows us to establish the pseudogap in electron-doped cuprates as a precursor to the incipient antiferromagnetic order even when long-range antiferromagnetic correlations are not established, as in the case of optimal doping.

A timely look into electron-phonon coupling: The coupling between electrons and phonons—lattice vibrations in solids—is responsible for macroscopic quantum phenomena such as superconductivity. Yet, experimentally measuring this coupling as a function of momentum and for a particular phonon mode is tricky. Na et al. used time- and angle-resolved photoemission spectroscopy to excite electrons in graphite and monitor their decay, which was accompanied by the release of phonons. The time constants of these decay processes provided direct information on electron-phonon couplings in this system. Science , this issue p. 1231

Strain-induced Landau levels in wafer-scale graphene at room temperature are studied using momentum-resolved spectroscopy.

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution—which is highly desirable for many TR-ARPES studies—while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity, realizing a practical source for TR-ARPES that achieves a flux of over 1011 photons/s delivered to the sample, operates over a range of 8–40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe2, as well as TR-ARPES studies on graphite.