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The resolution of angle-resolved photoelectron spectroscopy (ARPES) in three-dimensional (3D) momentum k is fundamentally limited by ill defined surface-perpendicular wave vector k⊥ associated with the finite photoelectron mean free path. Pushing ARPES into the soft-x-ray energy region sharpens the k⊥ definition, allowing accurate electronic structure investigations in 3D materials. We apply soft-x-ray ARPES to explore the 3D electron realm in a paradigm transition metal dichalcogenide VSe2. Essential to break through the dramatic loss of the valence band photoexcitation cross section at soft-x-ray energies is the advanced photon flux performance of our synchrotron instrumentation. By virtue of the sharp 3D momentum definition, the soft-x-ray ARPES experimental band structure and Fermi surface of VSe2 show a textbook clarity. We identify pronounced 3D warping of the Fermi surface and show that its concomitant nesting acts as the precursor for the exotic 3D charge-density waves in VSe2. Our results demonstrate the immense potential of soft-x-ray ARPES to explore details of 3D electronic structure. [ABSTRACT FROM AUTHOR]

We show with systematic photoemission spectroscopy and scanning tunneling spectroscopy data that a spin helical surface state appears on the (110) surface of noncentrosymmetric, three-dimensional HgTe. The topological surface state in HgTe exhibits sharp, linear dispersion without κz variation, as well as clear, left-right imbalanced spin polarization and circular dichroism. Chemical gating by alkali metal deposition on the surface causes the unexpected opening and/or increase of a surface insulating gap without changing its topological property. Such an unusual behavior we uncover in three-dimensional HgTe sheds light on a convenient control of the Fermi surface and quantum transport in a topological insulator. [ABSTRACT FROM AUTHOR]

Fractionalization of an electronic quasiparticle into spin, charge, and orbital parts is a fundamental and characteristic property of interacting electrons in one dimension. However, real materials are never strictly one dimensional and the fractionalization phenomena are hard to observe. Here we studied the spin and orbital excitations of the anisotropic ladder material CaCu2O3, whose electronic structure is not one dimensional. Combining high-resolution resonant inelastic x-ray scattering experiments with theoretical model calculations, we show that (i) spin-orbital fractionalization occurs in CaCu2O3 along the leg direction x through the xz orbital channel as in a 1D system, and (ii) no fractionalization is observed for the xy orbital, which extends in both leg and rung direction, contrary to a 1D system. We conclude that the directional character of the orbital hopping can select different degrees of dimensionality. Using additional model calculations, we show that spin-orbital separation is generally far more robust than the spin-charge separation. This is not only due to the already mentioned selection realized by the orbital hopping, but also due to the fact that spinons are faster than the orbitons. [ABSTRACT FROM AUTHOR]

(Ga,Mn)As is a paradigm of a diluted magnetic semiconductor which shows ferromagnetism induced by doped hole carriers. With a few controversial models emerging from numerous experimental and theoretical studies, the mechanism of the ferromagnetism in (Ga,Mn)As still remains a puzzling enigma. In this article, we use soft x-ray angle-resolved photoemission spectroscopy to positively identify the ferromagnetic Mn 3d-derived impurity band (IB) in (Ga,Mn)As. The band appears dispersionless and hybridized with the light-hole band of the host GaAs. These findings conclude the picture of the valence-band structure of (Ga,Mn)As disputed for more than a decade. The nondispersive character of the IB and its location in vicinity of the valence-band maximum indicate that the Mn 3d-derived IB is formed as a split-off Mn-impurity state predicted by the Anderson impurity model. Responsible for the ferromagnetism is predominantly the transport of hole carriers in the IB. [ABSTRACT FROM AUTHOR]

Taking spinon excitations in the quantum antiferromagnet CaCu2O3 as an example, we demonstrate that femtosecond dynamics of magnetic electronic excitations can be probed by direct resonant inelastic x-ray scattering (RIXS). To this end, we isolate the contributions of single and double spin-flip excitations in experimental RIXS spectra, identify the physical mechanisms that cause them, and determine their respective time scales. By comparing theory and experiment, we find that double spin flips need a finite amount of time to be generated, rendering them sensitive to the core-hole lifetime, whereas single spin flips are, to a very good approximation, independent of it. This shows that RIXS can grant access to time-domain dynamics of excitations and illustrates how RIXS experiments can distinguish between excitations in correlated electron systems based on their different time dependence. [ABSTRACT FROM AUTHOR]

We report a high-resolution resonant inelastic soft x-ray scattering study of the quantum magnetic spin- chain materials Li2CuO2 and CuGeO3. By tuning the incoming photon energy to the oxygen K edge, a strong excitation around 3.5 eV energy loss is clearly resolved for both materials. Comparing the experimental data to many-body calculations, we identify this excitation as a Zhang-Rice singlet exciton on neighboring CuO4 plaquettes. We demonstrate that the strong temperature dependence of the inelastic scattering related to this high-energy exciton enables us to probe short-range spin correlations on the 1 meV scale with outstanding sensitivity. [ABSTRACT FROM AUTHOR]

BiTel has a layered and noncentrosymmetric structure where strong spin-orbit interaction leads to a giant Rashba spin splitting in the bulk bands. We present direct measurements of the bulk band structure obtained with soft x-ray angle-resolved photoemission (ARPES), revealing the three-dimensional Fermi surface. The observed spindle torus shape bears the potential for a topological transition in the bulk by hole doping. Moreover, the bulk electronic structure is clearly disentangled from the two-dimensional surface electronic structure by means of high-resolution and spin-resolved ARPES measurements in the ultraviolet regime. All findings are supported by ab initio calculations [ABSTRACT FROM AUTHOR]

The important source of interface conductivity in LaAlO3/SrTiO3 heterostructures, the Ti 3d carriers, is probed with resonant inelastic x-ray scattering at the Ti 2p3/2 edge of epitaxially grown superlattices. We reveal unambiguously the generation of both localized and delocalized Ti 3d carriers as a result of the built-up heterointerface. Furthermore, we determine that the interface Ti3+O6 octahedra are orthorhombically distorted and quantify the crystal-field splitting energies. We argue that for as-grown superlattices, both types of Ti 3d carriers originate mainly from oxygen vacancies, whereas for fully oxidized samples they result from electronic reconstruction. [ABSTRACT FROM AUTHOR]

Resonant inelastic x-ray scattering (RIXS) experiments performed at the oxygen K edge on the iridate perovskites Sr2 IrO4 and Sr3 Ir2 O7 reveal a sequence of well-defined dispersive modes over the energy range up to ~0.8 eV . The momentum dependence of these modes and their variation with the experimental geometry allows us to assign each of them to specific collective magnetic and/or electronic excitation processes, including single and bimagnons, and spin-orbit and electron-hole excitons. We thus demonstrate that dispersive magnetic and electronic excitations are observable at the O K edge in the presence of the strong spin-orbit coupling in the 5 d shell of iridium and strong hybridization between Ir 5 d and O 2 p orbitals, which confirm and expand theoretical expectations. More generally, our results establish the utility of O K-edge RIXS for studying the collective excitations in a range of 5 d materials that are attracting increasing attention due to their novel magnetic and electronic properties. Especially, the strong RIXS response at O K edge opens up the opportunity for investigating collective excitations in thin films and heterostructures fabricated from these materials. [ABSTRACT FROM AUTHOR]

The electronic structure of α-Sn (001) thin films strained compressively in-plane was studied both experimentally and theoretically. A new topological surface state (TSS) located entirely within the gapless projected bulk bands is revealed by ab initio-based tight-binding calculations as well as directly accessed by soft x-ray angle-resolved photoemission. The topological character of this state, which is a surface resonance, is confirmed by unravelling the band inversion and by calculating the topological invariants. In agreement with experiment, electronic structure calculations show the maximum density of states in the subsurface region, while the already established TSS near the Fermi level is strongly localized at the surface. Such varied behavior is explained by the differences in orbital composition between the specific TSS and its associated bulk states, i.e., their hybridization, respectively. [ABSTRACT FROM AUTHOR]

We present an experimental study of the local and collective magnetism of EuFe2As2 that is isostructural with the high-temperature superconductor parent compound BaFe2As2. In contrast to BaFe2As2, where only Fe spins order, EuFe2As2 has an additional magnetic transition below 20 K due to the ordering of the Eu2+ spins (J=7/2, with L=0 and S=7/2) in an A-type antiferromagnetic texture (ferromagnetic layers stacked antiferromagnetically). This may potentially affect the FeAs layer and its local and correlated magnetism. FeKβ x-ray emission experiments on EuFe2As2 single crystals reveal a local magnetic moment of 1.3±0.15μB at 15 K that increases slightly to 1.45±0.15μB at 300 K. Resonant inelastic x-ray scattering experiments performed on the same crystals show dispersive broad (in energy) magnetic excitations along (0,0)→(1,0) and (0,0)→(1,1) with a bandwidth on the order of 170-180 meV. These results on local and collective magnetism are in line with other parent compounds of the AFe2As2 series (A=Ba, Ca, and Sr), especially the well-characterized BaFe2As2. Thus, our experiments lead us to the conclusion that the effect of the high magnetic moment of Eu on the magnitude of both the Fe local magnetic moment and spin excitations is small and confined to low-energy excitations. [ABSTRACT FROM AUTHOR]

Cuprate materials, such as those hosting high-temperature superconductivity, represent a famous class of materials where the correlations between the strongly entangled charges and spins produce complex phase diagrams. Several years ago, the Zhang-Rice singlet was proposed as a natural quasiparticle in hole-doped cuprates. The occurrence and binding energy of this quasiparticle, consisting of a pair of bound holes with antiparallel spins on the same CuO4 plaquette, depends on the local electronic interactions, which are fundamental quantities for understanding the physics of the cuprates. Here, we employ state-of-the-art resonant inelastic x-ray scattering (RIXS) to probe the correlated physics of the CuO4 plaquettes in the quasi-one-dimensional chain cuprate Li2CuO2. By tuning the incoming photon energy to the O K edge, we populate bound states related to the Zhang-Rice quasiparticles in the RIXS process. Both intra- and interchain Zhang-Rice singlets are observed and their occurrence is shown to depend on the nearest-neighbor spin-spin correlations, which are readily probed in this experiment. We also extract the binding energy of the Zhang-Rice singlet and identify the Zhang-Rice triplet excitation in the RIXS spectra. [ABSTRACT FROM AUTHOR]

We study the fate of the surface states of Bi2Se3 under disorder with strength larger than the bulk gap, caused by neon sputtering and nonmagnetic adsorbates. We find that neon sputtering introduces strong but dilute defects, which can be modeled by a unitary impurity distribution, whereas adsorbates, such as water vapor or carbon monoxide, are best described by Gaussian disorder. Remarkably, these two disorder types have a dramatically different effect on the surface states. Our soft x-ray angle-resolved photoemission spectroscopy (ARPES) measurements combined with numerical simulations show that unitary surface disorder pushes the Dirac state to inward quintuplet layers, burying it below an insulating surface layer. As a consequence, the surface spectral function becomes weaker but retains its quasiparticle peak. This is in contrast to Gaussian disorder, which smears out the quasiparticle peak completely. At the surface of Bi2Se3, neon sputtering adds additional unitary scatterers to the Gaussian disorder of the adsorbates. Since the introduced unitary disorder pushes the surface state to inward layers, the effects of Gaussian disorder are reduced. As a result the ARPES signal becomes sharper upon sputtering. [ABSTRACT FROM AUTHOR]

We have used resonant inelastic x-ray scattering (RIXS) and dynamical susceptibility calculations to study the magnetic excitations in NaFe1-xCoxAs (x=0, 0.03, and 0.08). Despite a relatively low ordered magnetic moment, collective magnetic modes are observed in parent compounds (x=0) and persist in optimally (x=0.03) and overdoped (x=0.08) samples. Their magnetic bandwidths are unaffected by doping within the range investigated. High-energy magnetic excitations in iron pnictides are robust against doping and present irrespectively of the ordered magnetic moment. Nevertheless, Co doping slightly reduces the overall magnetic spectral weight, differently from previous studies on hole-doped BaFe2As2, where it was observed constant. Finally, we demonstrate that the doping evolution of magnetic modes is different for the dopants being inside or outside the Fe-As layer. [ABSTRACT FROM AUTHOR]

We use resonant inelastic x-ray scattering (RIXS) at the Fe-L_{3} edge to study the spin excitations of uniaxial-strained and unstrained FeSe_{1-x}S_{x} (0≤x≤0.21) samples. The measurements on unstrained samples reveal dispersive spin excitations in all doping levels, which show only minor doping dependence in energy dispersion, lifetime, and intensity, indicating that high-energy spin excitations are only marginally affected by sulfur doping. RIXS measurements on uniaxial-strained samples reveal that the high-energy spin-excitation anisotropy observed previously in FeSe is also present in the doping range 0200  K in x=0.18 and reaches a maximum around the nematic quantum critical doping (x_{c}≈0.17). Since the spin-excitation anisotropy directly reflects the existence of nematic spin correlations, our results indicate that high-energy nematic spin correlations pervade the regime of nematicity in the phase diagram and are enhanced by the nematic quantum criticality. These results emphasize the essential role of spin fluctuations in driving electronic nematicity and highlight the capability of uniaxial strain in tuning spin excitations in quantum materials hosting strong magnetoelastic coupling and electronic nematicity.

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal. We identify all bulk branches of a higher-fold chiral fermion for the first time, critically important for allowing us to explore unique Fermi arc surface states in multiple interband gaps, which exhibit an emergent ladder structure. Through designer chemical gating of the samples in combination with our measurements, we uncover an unprecedented multigap bulk boundary correspondence. Our demonstration of multigap electronic topology will propel future research on unconventional topological responses.

Fractionalization of an electronic quasiparticle into spin, charge, and orbital parts is a fundamental and characteristic property of interacting electrons in one dimension. However, real materials are never strictly one dimensional and the fractionalization phenomena are hard to observe. Here we studied the spin and orbital excitations of the anisotropic ladder material CaCu_{2}O_{3}, whose electronic structure is not one dimensional. Combining high-resolution resonant inelastic x-ray scattering experiments with theoretical model calculations, we show that (i) spin-orbital fractionalization occurs in CaCu_{2}O_{3} along the leg direction x through the xz orbital channel as in a 1D system, and (ii) no fractionalization is observed for the xy orbital, which extends in both leg and rung direction, contrary to a 1D system. We conclude that the directional character of the orbital hopping can select different degrees of dimensionality. Using additional model calculations, we show that spin-orbital separation is generally far more robust than the spin-charge separation. This is not only due to the already mentioned selection realized by the orbital hopping, but also due to the fact that spinons are faster than the orbitons.

Taking spinon excitations in the quantum antiferromagnet CaCu2O3 as an example, we demonstrate that femtosecond dynamics of magnetic electronic excitations can be probed by direct resonant inelastic x-ray scattering (RIXS). To this end, we isolate the contributions of single and double spin-flip excitations in experimental RIXS spectra, identify the physical mechanisms that cause them, and determine their respective time scales. By comparing theory and experiment, we find that double spin flips need a finite amount of time to be generated, rendering them sensitive to the core-hole lifetime, whereas single spin flips are, to a very good approximation, independent of it. This shows that RIXS can grant access to time-domain dynamics of excitations and illustrates how RIXS experiments can distinguish between excitations in correlated electron systems based on their different time dependence.

We report a high-resolution resonant inelastic soft x-ray scattering study of the quantum magnetic spin-chain materials Li(2)CuO(2) and CuGeO(3). By tuning the incoming photon energy to the oxygen K edge, a strong excitation around 3.5 eV energy loss is clearly resolved for both materials. Comparing the experimental data to many-body calculations, we identify this excitation as a Zhang-Rice singlet exciton on neighboring CuO(4) plaquettes. We demonstrate that the strong temperature dependence of the inelastic scattering related to this high-energy exciton enables us to probe short-range spin correlations on the 1 meV scale with outstanding sensitivity.

Inelastic x-ray scattering spectra excited at the 1s(-1)π* resonance of gas phase O2 have been recorded with an overall energy resolution that allows for well-resolved vibrational progressions. The nuclear wave packet dynamics in the intermediate state is reflected in vibrational excitations of the electronic ground state, and by fine-tuning the excitation energy the dissociation dynamics in the predissociative B'(3)Πg final state is controlled.