Chirality-Driven Orbital Angular Momentum and Circular Dichroism in CoSi.

Chiral crystals and molecules were recently predicted to form an intriguing platform for unconventional orbital physics. Here, we report the observation of chirality-driven orbital textures in the bulk electronic structure of CoSi, a prototype member of the cubic B20 family of chiral crystals. Using circular dichroism in soft x-ray angle-resolved photoemission, we demonstrate the formation of a bulk orbital-angular-momentum texture and monopolelike orbital-momentum locking that depends on crystal handedness. We introduce the intrinsic chiral circular dichroism, icCD, as a differential photoemission observable and a natural probe of chiral electron states. Our findings render chiral crystals promising for spin-orbitronics applications.

New Measurement Resolves Key Astrophysical Fe XVII Oscillator Strength Problem.

One of the most enduring and intensively studied problems of x-ray astronomy is the disagreement of state-of-the art theory and observations for the intensity ratio of two Fe XVII transitions of crucial value for plasma diagnostics, dubbed 3C and 3D. We unravel this conundrum at the PETRA III synchrotron facility by increasing the resolving power 2.5 times and the signal-to-noise ratio thousandfold compared with our previous work. The Lorentzian wings had hitherto been indistinguishable from the background and were thus not modeled, resulting in a biased line-strength estimation. The present experimental oscillator-strength ratio R_{exp}=f_{3C}/f_{3D}=3.51(2)_{stat}(7)_{sys} agrees with our state-of-the-art calculation of R_{th}=3.55(2), as well as with some previous theoretical predictions. To further rule out any uncertainties associated with the measured ratio, we also determined the individual natural linewidths and oscillator strengths of 3C and 3D transitions, which also agree well with the theory. This finally resolves the decades-old mystery of Fe XVII oscillator strengths.

Charge Density Waves in Electron-Doped Molybdenum Disulfide.

We present the discovery of a charge density wave (CDW) ground state in heavily electron-doped molybdenum disulfide (MoS2). This is the first observation of a CDW in any d2 (column 6) transition metal dichalcogenide (TMD). The band structure of MoS2 is distinct from the d0 and d1 TMDs in which CDWs have been previously observed, facilitating new insight into CDW formation. We demonstrate a metal-insulator transition at 85 K, a 25 meV gap at the Fermi level, and two distinct CDW modulations, (2√3 × 2√3) R30° and 2 × 2, attributable to Fermi surface nesting (FSN) and electron-phonon coupling (EPC), respectively. This simultaneous exhibition of FSN and EPC CDW modulations is unique among observations of CDW ground states, and we discuss this in the context of band folding. Our observations provide a route toward the resolution of controversies surrounding the origin of CDW modulations in TMDs.

Characterization of the Percival detector with soft X-rays.

In this paper the back-side-illuminated Percival 2-Megapixel (P2M) detector is presented, along with its characterization by means of optical and X-ray photons. For the first time, the response of the system to soft X-rays (250 eV to 1 keV) is presented. The main performance parameters of the first detector are measured, assessing the capabilities in terms of noise, dynamic range and single-photon discrimination capability. Present limitations and coming improvements are discussed.

Itinerant ferromagnetism of the Pd-terminated polar surface of PdCoO2.

The ability to modulate the collective properties of correlated electron systems at their interfaces and surfaces underpins the burgeoning field of "designer" quantum materials. Here, we show how an electronic reconstruction driven by surface polarity mediates a Stoner-like magnetic instability to itinerant ferromagnetism at the Pd-terminated surface of the nonmagnetic delafossite oxide metal PdCoO2 Combining angle-resolved photoemission spectroscopy and density-functional theory calculations, we show how this leads to a rich multiband surface electronic structure. We find similar surface state dispersions in PdCrO2, suggesting surface ferromagnetism persists in this sister compound despite its bulk antiferromagnetic order.

Direct 2D spatial-coherence determination using the Fourier-analysis method: multi-parameter characterization of the P04 beamline at PETRA III.

We present a systematic 2D spatial-coherence analysis of the soft-X-ray beamline P04 at PETRA III for various beamline configurations. The influence of two different beam-defining apertures on the spatial coherence properties of the beam is discussed and optimal conditions for coherence-based experiments are found. A significant degradation of the spatial coherence in the vertical direction has been measured and sources of this degradation are identified and discussed. The Fourier-analysis method, which gives fast and simple access to the 2D spatial coherence function of the X-ray beam, is used for the experiment. Here, we exploit the charge scattering of a disordered nanodot sample allowing the use of arbitrary X-ray photon energies with this method.

Enabling time-resolved 2D spatial-coherence measurements using the Fourier-analysis method with an integrated curved-grating beam monitor.

Direct 2D spatial-coherence measurements are increasingly gaining importance at synchrotron beamlines, especially due to present and future upgrades of synchrotron facilities to diffraction-limited storage rings. We present a method to determine the 2D spatial coherence of synchrotron radiation in a direct and particularly simple way by using the Fourier-analysis method in conjunction with curved gratings. Direct photon-beam monitoring provided by a curved grating circumvents the otherwise necessary separate determination of the illuminating intensity distribution required for the Fourier-analysis method. Hence, combining these two methods allows for time-resolved spatial-coherence measurements. As a consequence, spatial-coherence degradation effects caused by beamline optics vibrations, which is one of the key issues of state-of-the-art X-ray imaging and scattering beamlines, can be identified and analyzed.

High Resolution Photoexcitation Measurements Exacerbate the Long-Standing Fe XVII Oscillator Strength Problem.

For more than 40 years, most astrophysical observations and laboratory studies of two key soft x-ray diagnostic 2p-3d transitions, 3C and 3D, in Fe XVII ions found oscillator strength ratios f(3C)/f(3D) disagreeing with theory, but uncertainties had precluded definitive statements on this much studied conundrum. Here, we resonantly excite these lines using synchrotron radiation at PETRA III, and reach, at a millionfold lower photon intensities, a 10 times higher spectral resolution, and 3 times smaller uncertainty than earlier work. Our final result of f(3C)/f(3D)=3.09(8)(6) supports many of the earlier clean astrophysical and laboratory observations, while departing by five sigmas from our own newest large-scale ab initio calculations, and excluding all proposed explanations, including those invoking nonlinear effects and population transfers.

Zone plates for angle-resolved photoelectron spectroscopy providing sub-micrometre resolution in the extreme ultraviolet regime.

This article reports on the fabrication and testing of dedicated Fresnel zone plates for use at the nano-ARPES branch of the I05-ARPES beamline of Diamond Light Source to perform angle-resolved photoelectron spectroscopy with sub-micrometre resolution in real space. The aim of the design was to provide high photon flux combined with sub-micrometre spot sizes. The focusing lenses were tested with respect to efficiency and spatial resolution in the extreme ultraviolet between 50 eV and 90 eV. The experimentally determined diffraction efficiencies of the zone plates are as high as 8.6% at 80 eV, and a real-space resolution of 0.4 µm was demonstrated. Using the zone-plate-based setup, monolayer flakes of the two-dimensional semiconductor WS2 were investigated. This work demonstrates that the local electronic structure can be obtained from an area of a few micrometres across a two-dimensional heterostructure.

Holstein polaron in a valley-degenerate two-dimensional semiconductor.

Two-dimensional (2D) crystals have emerged as a class of materials with tunable carrier density1. Carrier doping to 2D semiconductors can be used to modulate many-body interactions2 and to explore novel composite particles. The Holstein polaron is a small composite particle of an electron that carries a cloud of self-induced lattice deformation (or phonons)3-5, which has been proposed to play a key role in high-temperature superconductivity6 and carrier mobility in devices7. Here we report the discovery of Holstein polarons in a surface-doped layered semiconductor, MoS2, in which a puzzling 2D superconducting dome with the critical temperature of 12 K was found recently8-11. Using a high-resolution band mapping of charge carriers, we found strong band renormalizations collectively identified as a hitherto unobserved spectral function of Holstein polarons12-18. The short-range nature of electron-phonon (e-ph) coupling in MoS2 can be explained by its valley degeneracy, which enables strong intervalley coupling mediated by acoustic phonons. The coupling strength is found to increase gradually along the superconducting dome up to the intermediate regime, which suggests a bipolaronic pairing in the 2D superconductivity.

Disorder Quenching of the Charge Density Wave in ZrTe_{3}.

The charge density wave (CDW) in ZrTe_{3} is quenched in samples with a small amount of Te isoelectronically substituted by Se. Using angle-resolved photoemission spectroscopy we observe subtle changes in the electronic band dispersions and Fermi surfaces upon Se substitution. The scattering rates are substantially increased, in particular for the large three-dimensional Fermi surface sheet. The quasi-one-dimensional band is unaffected by the substitution and still shows a gap at low temperature, which starts to open from room temperature. Long-range order is, however, absent in the electronic states as in the periodic lattice distortion. The competition between superconductivity and the CDW is thus linked to the suppression of long-range order of the CDW.

Spin Orientation of Two-Dimensional Electrons Driven by Temperature-Tunable Competition of Spin-Orbit and Exchange-Magnetic Interactions.

Finding ways to create and control the spin-dependent properties of two-dimensional electron states (2DESs) is a major challenge for the elaboration of novel spin-based devices. Spin-orbit and exchange-magnetic interactions (SOI and EMI) are two fundamental mechanisms that enable access to the tunability of spin-dependent properties of carriers. The silicon surface of HoRh2Si2 appears to be a unique model system, where concurrent SOI and EMI can be visualized and controlled by varying the temperature. The beauty and simplicity of this system lie in the 4f moments, which act as a multiple tuning instrument on the 2DESs, as the 4f projections parallel and perpendicular to the surface order at essentially different temperatures. Here we show that the SOI locks the spins of the 2DESs exclusively in the surface plane when the 4f moments are disordered: the Rashba-Bychkov effect. When the temperature is gradually lowered and the system experiences magnetic order, the rising EMI progressively competes with the SOI leading to a fundamental change in the spin-dependent properties of the 2DESs. The spins rotate and reorient toward the out-of-plane Ho 4f moments. Our findings show that the direction of the spins and the spin-splitting of the two-dimensional electrons at the surface can be manipulated in a controlled way by using only one parameter: the temperature.

Nonadiabatic Kohn Anomaly in Heavily Boron-Doped Diamond.

We report evidence of a nonadiabatic Kohn anomaly in boron-doped diamond, using a joint theoretical and experimental analysis of the phonon dispersion relations. We demonstrate that standard calculations of phonons using density-functional perturbation theory are unable to reproduce the dispersion relations of the high-energy phonons measured by high-resolution inelastic x-ray scattering. On the contrary, by taking into account nonadiabatic effects within a many-body field-theoretic framework, we obtain excellent agreement with our experimental data. This result indicates a breakdown of the Born-Oppenheimer approximation in the phonon dispersion relations of boron-doped diamond.

Observation of time-reversal symmetry breaking in the band structure of altermagnetic RuO2.

Altermagnets are an emerging elementary class of collinear magnets. Unlike ferromagnets, their distinct crystal symmetries inhibit magnetization while, unlike antiferromagnets, they promote strong spin polarization in the band structure. The corresponding unconventional mechanism of time-reversal symmetry breaking without magnetization in the electronic spectra has been regarded as a primary signature of altermagnetism but has not been experimentally visualized to date. We directly observe strong time-reversal symmetry breaking in the band structure of altermagnetic RuO2 by detecting magnetic circular dichroism in angle-resolved photoemission spectra. Our experimental results, supported by ab initio calculations, establish the microscopic electronic structure basis for a family of interesting phenomena and functionalities in fields ranging from topological matter to spintronics, which are based on the unconventional time-reversal symmetry breaking in altermagnets.

Anharmonicity due to electron-phonon coupling in magnetite.

We present the results of inelastic x-ray scattering for magnetite and analyze the energies and widths of the phonon modes with different symmetries in a broad range of temperature 125 < T < 293 K. The phonon modes with X(4) and Δ(5) symmetries broaden in a nonlinear way with decreasing T when the Verwey transition is approached. It is found that the maxima of phonon widths occur away from high-symmetry points, which suggests the incommensurate character of critical fluctuations. Strong phonon anharmonicity induced by electron-phonon coupling is discovered by a combination of these experimental results with ab initio calculations which take into account local Coulomb interactions at Fe ions. It (i) explains observed anomalous phonon broadening and (ii) demonstrates that the Verwey transition is a cooperative phenomenon which involves a wide spectrum of phonons coupled to the electron charge fluctuations condensing in the low-symmetry phase.

Microstructure effects on the phase transition behavior of a prototypical quantum material.

Materials with insulator-metal transitions promise advanced functionalities for future information technology. Patterning on the microscale is key for miniaturized functional devices, but material properties may vary spatially across microstructures. Characterization of these miniaturized devices requires electronic structure probes with sufficient spatial resolution to understand the influence of structure size and shape on functional properties. The present study demonstrates the use of imaging soft X-ray absorption spectroscopy with a spatial resolution better than 2 [Formula: see text]m to study the insulator-metal transition in vanadium dioxide thin-film microstructures. This novel technique reveals that the transition temperature for the conversion from insulating to metallic vanadium dioxide is lowered by 1.2 K ± 0.4 K close to the structure edges compared to the center. Facilitated strain release during the phase transition is discussed as origin of the observed behavior. The experimental approach enables a detailed understanding of how the electronic properties of quantum materials depend on their patterning at the micrometer scale.

Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb2O6.

Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6 which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.

Time-reversal symmetry breaking type-II Weyl state in YbMnBi2.

Spectroscopic detection of Dirac and Weyl fermions in real materials is vital for both, promising applications and fundamental bridge between high-energy and condensed-matter physics. While the presence of Dirac and noncentrosymmetric Weyl fermions is well established in many materials, the magnetic Weyl semimetals still escape direct experimental detection. In order to find a time-reversal symmetry breaking Weyl state we design two materials and present here experimental and theoretical evidence of realization of such a state in one of them, YbMnBi2. We model the time-reversal symmetry breaking observed by magnetization and magneto-optical microscopy measurements by canted antiferromagnetism and find a number of Weyl points. Using angle-resolved photoemission, we directly observe two pairs of Weyl points connected by the Fermi arcs. Our results not only provide a fundamental link between the two areas of physics, but also demonstrate the practical way to design novel materials with exotic properties.

Boron-Doped Graphene Nanoribbons: Electronic Structure and Raman Fingerprint.

We investigate the electronic and vibrational properties of bottom-up synthesized aligned armchair graphene nanoribbons of N = 7 carbon atoms width periodically doped by substitutional boron atoms (B-7AGNRs). Using angle-resolved photoemission spectroscopy and density functional theory calculations, we find that the dopant-derived valence and conduction band states are notably hybridized with electronic states of Au substrate and spread in energy. The interaction with the substrate leaves the bands with pure carbon character rather unperturbed. This results in an identical effective mass of ≈0.2 m0 for the next-highest valence band compared with pristine 7AGNRs. We probe the phonons of B-7AGNRs by ultrahigh-vacuum (UHV) Raman spectroscopy and reveal the existence of characteristic splitting and red shifts in Raman modes due to the presence of substitutional boron atoms. Comparing the Raman spectra for three visible lasers (red, green, and blue), we find that interaction with gold suppresses the Raman signal from B-7AGNRs and the energy of the green laser (2.33 eV) is closer to the resonant E22 transition. The hybridized electronic structure of the B-7AGNR-Au interface is expected to improve electrical characteristics of contacts between graphene nanoribbon and Au. The Raman fingerprint allows the easy identification of B-7AGNRs, which is particularly useful for device fabrication.

A novel artificial condensed matter lattice and a new platform for one-dimensional topological phases.

Engineered lattices in condensed matter physics, such as cold-atom optical lattices or photonic crystals, can have properties that are fundamentally different from those of naturally occurring electronic crystals. We report a novel type of artificial quantum matter lattice. Our lattice is a multilayer heterostructure built from alternating thin films of topological and trivial insulators. Each interface within the heterostructure hosts a set of topologically protected interface states, and by making the layers sufficiently thin, we demonstrate for the first time a hybridization of interface states across layers. In this way, our heterostructure forms an emergent atomic chain, where the interfaces act as lattice sites and the interface states act as atomic orbitals, as seen from our measurements by angle-resolved photoemission spectroscopy. By changing the composition of the heterostructure, we can directly control hopping between lattice sites. We realize a topological and a trivial phase in our superlattice band structure. We argue that the superlattice may be characterized in a significant way by a one-dimensional topological invariant, closely related to the invariant of the Su-Schrieffer-Heeger model. Our topological insulator heterostructure demonstrates a novel experimental platform where we can engineer band structures by directly controlling how electrons hop between lattice sites.