In doped Hund's metals, such as the iron-based superconductors, effects like charge doping and chemical pressure are often considered the dominant factors. Partial chemical substitution, however, inevitably introduces disorder. Here, we investigate spin excitations in Ba( Fe 1 − x Cr x ) 2 As 2 (CrBFA) by high-resolution resonant inelastic x-ray scattering for samples with x = 0 , 0.035 , and 0.085 . In CrBFA, Cr acts as a hole dopant, but also introduces localized spins that compete with Fe-derived magnetic excitations. We found that the Fe-derived magnetic excitations are softened and damped, becoming overdamped for x = 0.085 . At this doping level, complementary angle-resolved photoemission spectroscopy measurements show increased electronic localization and a suppression of the nematic d x z / d y z band splitting present in the parent compound. We thus propose a localized spin model that explicitly incorporates substitutional disorder and Cr local moments, successfully reproducing our key observations. Our findings reveal a case where disorder dominates over charge doping in the case of a Hund's metal.

Excitons are key quasiparticles determining the optical properties of solids. As such, they can be utilized to coherently control the electronic structure of materials using optical femtosecond pulses. Identifying the decoherence mechanism during the early non-equilibrium dynamics is crucial to achieve light-induced band-structure engineering in semiconductors. Here, we generate excitons in the direct band gap semiconductor black phosphorus with a resonant mid-infrared photoexcitation. Using time- and angle-resolved photoemission spectroscopy, we track their complex ultrafast dynamics on the few-picosecond time scale. We develop a quantum-kinetic theoretical framework to model the decoherence of excitons into dark excitons via phonon scattering. By combining simulation and experiment, we quantify key parameters describing the early dynamics of the excitons. Our work highlights phonon-mediated intravalley scattering as a fundamental limitation for coherent exciton phenomena in single-valley semiconductors.

In doped Hund's metals, such as the iron-based superconductors, effects like charge doping and chemical pressure are often considered the dominant factors. Partial chemical substitution, however, inevitably introduces disorder. Here, we investigate spin excitations in Ba(Fe1-xCrx)2As2 (CrBFA) by high-resolution resonant inelastic x-ray scattering for samples with x = 0, 0.035, and 0.085. In CrBFA, Cr acts as a hole dopant, but also introduces localized spins that compete with Fe-derived magnetic excitations. We found that the Fe-derived magnetic excitations are softened and damped, becoming overdamped for x = 0.085. At this doping level, complementary angle-resolved photoemission spectroscopy measurements show increased electronic localization and a suppression of the nematic dxz/dyz band splitting present in the parent compound. We thus propose a localized spin model that explicitly incorporates substitutional disorder and Cr local moments, successfully reproducing our key observations. Our findings reveal a case where disorder dominates over charge doping in the case of a Hund's metal.

The filling of the large van der Waals gap in Transition Metal Dichalcogenides (TMDs) often leads to lattice and electronic instabilities, which prelude the onset of a rich phenomenology. Here, we investigate the electronic structure of the TMDs ZrTe_2 and Ni-intercalated ZrTe_2 (Ni_xZrTe_2, x≈ 0.05) employing angle-resolved photoemission spectroscopy (ARPES). We readily identify in Ni_xZrTe_2 two flat bands, most likely associated with localized Ni-derived 3d-states, at about ≈-0.7 eV and ≈-1.2 eV in binding energy. The presence of these flat bands is observed for all temperatures (T) in our study. More significantly, at low-T, we identify an electronic structure reconstruction in Ni_xZrTe_2, which halves the electronic periodicity along the k_z direction. This is reminiscent of a commensurate band folding with wave-vector q=(0,0,π). Together with previous results from macroscopic measurements, namely heat capacity and resistivity, our findings suggest that Ni intercalation drives a structural instability at T^*=287 K, which causes the observed electronic band reconstruction. Our findings invite further investigation into the structural properties of ZrTe_2 and of the intercalated and defect-engineered versions of this material.

The low-energy electronic structure of materials is crucial to understanding and modeling their physical properties. Angle-resolved photoemission spectroscopy (ARPES) is the best experimental technique to measure this electronic structure, but its interpretation can be delicate. Here we use a combination of density functional theory (DFT) and one-step model of photoemission to decipher the soft x-ray ARPES spectra of the quaternary borocarbide superconductor YNi 2 B 2 C. Our analysis reveals the presence of moderate electronic correlations beyond the semilocal DFT within the generalized gradient approximation. We show that DFT and the full potential Korringa-Kohn-Rostoker method combined with the dynamical mean field theory (DFT+DMFT) with average Coulomb interaction U = 3.0 eV and the exchange energy J = 0.9 eV applied to the Ni d -states are necessary for reproducing the experimentally observed SX-ARPES spectra.

The ferroelectric semiconductor α-GeTe(111) has attracted significant attention in the last decade due to its unique properties, with extensive studies focusing on its occupied electronic bandstructure. In contrast, its unoccupied states - particularly those near the conduction band minimum - remain largely unexplored. In an effort to characterize those states, we surprisingly observe three image potential states (IPS) in α-GeTe(111) extending up to 0.8 eV above the vacuum level. Using time and angle-resolved photoemission spectroscopy, we resolve the full parabolic dispersions of the first three IPS and determine their binding energies. Our analysis, combined with Bloch spectral function calculations, reveals that the unexpected persistence of IPS above the vacuum level originates from strong dipole transitions and the presence of large electron reservoirs in GeTe.

Metal-assisted exfoliation of two-dimensional (2D) materials has emerged as an efficient route to isolating large-area monolayer crystals, yet the influence of the supporting metal substrate on their intrinsic properties remains poorly understood. Here, we demonstrate successful gold-assisted exfoliation of monolayer IrTe_2 up to the millimeter scale. Angle-resolved photoemission spectroscopy (ARPES), combined with first-principles calculations, reveals that the low-energy electronic structure closely resembles that of a freestanding monolayer 1T-IrTe_2. We find that quasi-covalent hybridization together with substrate-induced strain leads to only modest modifications of the electronic bands. Although strain contributes to phase stability, it is essentially hybridization that drives the stabilization of the 1T-phase of the monolayer IrTe_2 by suppressing stripe-ordered phase transitions. These results establish gold-assisted exfoliation as a robust route to prepare a large-area monolayer IrTe_2 and highlight the role of metal-substrate interaction in engineering 2D materials with tailored structural phases.

Resonant inelastic x-ray scattering (RIXS) can probe electron-hole excitations in excitonic insulators (EIs) which are realized by Coulomb attractive interaction between electrons and holes in semimetals or narrow gap semiconductors. In the present article, we review the exotic electronic state of an EI candidate Ta2NiSe5 which is probed by Ni 2p-3d RIXS as well as Ni 2p x-ray photoemission/absorption spectroscopy. The RIXS results on the exotic electronic state under the electron-hole and electron-lattice correlations suggest requirement of a new theoretical scheme which can describe itinerant electron-hole excitations and the localized charge-transfer excitations as well as the electron-lattice interaction.

alpha-GeTe(111) is a noncentrosymmetric ferroelectric (FE) material for which a significative lattice distortion combined with a strong spin-orbit interaction gives rise to giant Rashba split states in the bulk and at the surface, which have been intensively probed in the occupied valence states using static angle-resolved photoemission spectroscopy (ARPES). Nevertheless, its unoccupied conduction band structure remains unexplored, in particular the experimental determination of its electronic band gap across momentum space. Using time-resolved ARPES based on high-repetition rate and extreme ultraviolet femtosecond (fs) laser, we unveil the band structure of alpha-GeTe(111) in the full Brillouin zone, both in the valence and conduction states, as well as the exploration of its out-of-equilibrium dynamics. Our work confirms the semiconducting nature of alpha-GeTe(111) with a 0.85 eV indirect band gap, which provides an upper limit for comparison to density functional theory calculations. We finally reveal the dominant scattering mechanisms of photoexcited carriers during the out-of-equilibrium dynamics under fs light pulses.

We present a combined density functional theory (DFT), one-step model of photoemission, and soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) study of the electronic structure of the quaternary borocarbide superconductor YNi_2B_2C. Our analysis reveals the presence of moderate electronic correlations beyond the semilocal DFT within the generalized gradient approximation. We show that DFT and the full potential Korringa-Kohn-Rostoker method combined with the dynamical mean field theory (DFT+DMFT) with average Coulomb interaction U = 3.0 eV and the exchange energy J = 0.9 eV applied to the Ni d-states are necessary for reproducing the experimentally observed SX-ARPES spectra.

Competing interactions in low-dimensional materials can produce nearly degenerate electronic and structural phases. We investigate structural phase transitions in layered IrTe2 for which a number of potential transition mechanisms have been postulated. The spatial coexistence of multiple phases on the micron scale has prevented a detailed analysis of the electronic structure. By exploiting micro-angle-resolved photoemission spectroscopy obtained with synchrotron radiation we extract the electronic structure of the multiple structural phases in IrTe2 in order to address the mechanism underlying the phase transitions. We find direct evidence of lowered energy states that appear in the low-temperature phases, states previously predicted by ab initio calculations and extended here. Our results validate a proposed scenario of bonding and antibonding states as the driver of the phase transitions.

Heterostructures from complex oxides allow one to combine various electronic and magnetic orders as to induce new quantum states. A prominent example is the coupling between superconducting and magnetic orders in multilayers from high-Tc cuprates and manganites. A key role is played here by the interfacial CuO2 layer whose distinct properties remain to be fully understood. Here, we study with resonant inelastic X-ray scattering the magnon excitations of this interfacial CuO2 layer. In particular, we show that the underlying antiferromagnetic exchange interaction at the interface is strongly suppressed to J≈70 meV, when compared with J≈130 meV for the CuO2 layers away from the interface. Moreover, we observe an anomalous momentum dependence of the intensity of the interfacial magnon mode and show that it suggests that the antiferromagnetic order is accompanied by a particular kind of orbital order that yields a so-called altermagnetic state. Such a 2D altermagnet has recently been predicted to enable new spintronic applications and superconducting proximity effects.

Interlayer coupling is strongly implicated in the complex electronic properties of 1T-TaS2. Uniaxial strain engineering offers a route to modify this coupling in order to elucidate its interplay with the electronic structure and electronic correlations. Here, we employ angle -resolved photoemission spectroscopy (ARPES) to reveal the effect of uniaxial strain on the electronic structure in 1T-TaS2. The gap of the normally insulating ground state is significantly reduced, with a correlated flat band appearing close to the Fermi level. Temperature -dependent ARPES measurements reveal that the flat band only develops below the commensurate charge density wave (CCDW) transition, where interlayer dimerization produces a band insulator in unstrained samples. Electronic structure calculations suggest that the correlated flat band is stabilized by a modified interlayer coupling of the Ta dz2 electrons. Further hints of a strain -induced structural modification of the interlayer order are obtained from x-ray diffraction. Our combined approach provides critical input for understanding the complex phase diagram of this platform material for correlated physics.

The transition-metal dichalcogenide tantalum disulphide (1T-TaS2) hosts a commensurate charge density wave (CCDW) at temperatures below 165 K where it also becomes insulating. The low temperature CCDW phase can be driven into a metastable "mosaic" phase by means of either laser or voltage pulses, which shows a large density of CDW domain walls as well as a closing of the electronic band gap. The exact origins of this pulse-induced metallic mosaic are not yet fully understood. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we observe the occurrence of such a metallic mosaic phase on the surface of TaS2 without prior pulse excitation over continuous areas larger than 100 x 100 nm2 and macroscopic areas on the mil-limeter scale. We attribute the appearance of the mosaic phase to the presence of surface defects which cause the formation of the characteristic dense domain wall network. Based on our STM measurements, we further argue how the appearance of the metallic behavior in the mosaic phase could be explained by local stacking differences of the top layer. Thus we provide a potential avenue to explain the origin of the pulse-induced mosaic phase.

In the last 20 years, the technique of resonant inelastic X-ray scattering (RIXS) has been progressing at a high pace thanks to the concomitant development of instrumentation, synchrotron technology, and the theoretical description of the related fundamental process. In this article, we describe some recent aspects related to the fast progress of the RIXS technique and dedicate this article to the memory of Prof. Jean-Claude Dousse, from the University of Fribourg (Switzerland). We conclude this article by describing early experiments using time-resolved RIXS at X-ray free electron lasers and give perspectives on high-resolution and spatially-resolved RIXS.

Low-dimensional materials have remarkable properties that are distinct from their bulk counterparts. A paradigmatic example is Ising superconductivity that occurs in monolayer materials such as NbSe2 which show a strong violation of the Pauli limit. In monolayers, this occurs due to a combination of broken inversion symmetry and spin-orbit coupling that locks the spins of the electrons out-of-plane. Bulk NbSe2 is centrosymmetric and is therefore not an Ising superconductor. We show that bulk misfit compound superconductors, (LaSe)1.14(NbSe2) and (LaSe)1.14(NbSe2)2, comprised of monolayers and bilayers of NbSe2, exhibit unexpected Ising protection with a Pauli-limit violation comparable to monolayer NbSe2, despite formally having inversion symmetry. We study these misfit compounds using complementary experimental methods in combination with first-principles calculations. We propose theoretical mechanisms of how the Ising protection can survive in bulk materials. We show how some of these mechanisms operate in these bulk compounds due to a concerted effect of charge-transfer, defects, reduction of interlayer hopping, and stacking. This highlights how Ising superconductivity can, unexpectedly, arise in bulk materials, and possibly enable the design of bulk superconductors that are resilient to magnetic fields.

Using angle-resolved photoemission spectroscopy, combined with first principle and coupled self-consistent Poisson-Schrödinger calculations, we demonstrate that potassium (K) atoms adsorbed on the low-temperature phase of 1T-TiSe_{2} induce the creation of a two-dimensional electron gas (2DEG) and quantum confinement of its charge-density wave (CDW) at the surface. By further changing the K coverage, we tune the carrier density within the 2DEG that allows us to nullify, at the surface, the electronic energy gain due to exciton condensation in the CDW phase while preserving a long-range structural order. Our Letter constitutes a prime example of a controlled exciton-related many-body quantum state in reduced dimensionality by alkali-metal dosing.

Research on charge-density-wave (CDW) ordered transition-metal dichalcogenides continues to unravel new states of quantum matter correlated to the intertwined lattice and electronic degrees of freedom. Here, we report an inelastic x-ray scattering investigation of the lattice dynamics of the canonical CDW compound 2H-TaSe2 complemented by angle-resolved photoemission spectroscopy and density functional perturbation theory. Our results rule out the formation of a central-peak without full phonon softening for the CDW transition in 2H-TaSe2 and provide evidence for a novel precursor region above the CDW transition temperature TCDW, which is characterized by an overdamped phonon mode and not detectable in our photoemission experiments. Thus, 2H-TaSe2 exhibits structural before electronic static order and emphasizes the important lattice contribution to CDW transitions. Our ab-initio calculations explain the interplay of electron-phonon coupling and Fermi surface topology triggering the CDW phase transition and predict that the CDW soft phonon mode promotes emergent superconductivity near the pressure-driven CDW quantum critical point.

The ferroelectric semiconductor α-SnTe has been regarded as a topological crystalline insulator, and the dispersion of its surface states has been intensively measured with angle-resolved photoemission spectroscopy (ARPES) over the past decade. However, much less attention has been given to the impact of the ferroelectric transition on its electronic structure, and in particular on its bulk states. Here, we investigate the low-energy electronic structure of α-SnTe with ARPES and follow the evolution of the bulk-state Rashba splitting as a function of temperature, across its ferroelectric critical temperature of about Tc ≈ 110 K. Unexpectedly, we observe a persistent band splitting up to room temperature, which is consistent with an order–disorder contribution of local dipoles to the phase transition that requires the presence of fluctuating dipoles above Tc. We conclude that no topological surface state can occur under these conditions at the (111) surface of SnTe, at odds with recent literature.

Chemical substitution is commonly used to explore new ground states in materials, yet the role of disorder is often overlooked. In Mn-substituted BaFe$_{2}$As$_{2}$ (MnBFA), superconductivity (SC) is absent, despite being observed for nominal hole-doped phases. Instead, a glassy magnetic phase emerges, associated with the $S=5/2$ Mn local spins. In this work, we present a comprehensive investigation of the electronic structure of MnBFA using angle-resolved photoemission spectroscopy (ARPES). We find that Mn causes a small and orbital-specific reduction of the electron pockets, only partially disrupting nesting conditions. Based upon the analysis of the spectral properties, we observe, for all bands, an increase in the electronic scattering rate as a function of Mn content. This is interpreted as increasing band incoherence, which we propose as the primary contributor to the suppression of the magnetic order in MnBFA. This finding connects the MnBFA electronic band structure properties to the glassy magnetic behavior observed in these materials and suggests that SC is absent because of the collective magnetic impurity behavior that scatters the Fe-derived excitations. Additionally, our analysis shows that the binding energy ($E_{B}$) dependence of the imaginary part of the self-energy [$\text{Im}\Sigma(E_{B})$] is best described by a fractional scaling ($\text{Im}\Sigma(E_{B})\propto\sqrt{-E_{B}}$). These results indicate that Mn tunes MnBFA into an electronic disordered phase between the correlated Hund's metal in BaFe$_{2}$As$_{2}$ and the Hund's insulator in BaMn$_{2}$As$_{2}$.