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Angle-resolved photoelectron spectroscopy (ARPES) is the main experimental tool to explore electronic structure of solids resolved in the electron momentum k . Soft-X-ray ARPES (SX-ARPES), operating in a photon energy range around 1 keV, benefits from enhanced probing depth compared to the conventional VUV-range ARPES, and elemental/chemical state specificity achieved with resonant photoemission. These advantages make SX-ARPES ideally suited for buried heterostructure and impurity systems, which are at the heart of current and future electronics. These applications are illustrated here with a few pioneering results, including buried quantum-well states in semiconductor and oxide heterostructures, their bosonic coupling critically affecting electron transport, magnetic impurities in diluted magnetic semiconductors and topological materials, etc. High photon flux and detection efficiency are crucial for pushing the SX-ARPES experiment to these most photon-hungry cases.
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Taking advantage of the large electron escape depth of soft x-ray angle resolved photoemission spectroscopy we report electronic structure measurements of (111)-oriented [LaNiO3/LaMnO3] superlattices and LaNiO3 epitaxial films. For thin films we observe a 3D Fermi surface with an electron pocket at the Brillouin zone center and hole pockets at the zone vertices. Superlattices with thick nickelate layers present a similar electronic structure. However, as the thickness of the LaNiO3 is reduced the superlattices become insulating. These heterostructures do not show a marked redistribution of spectral weight in momentum space but exhibit a pseudogap of 50 meV.
The electronic structure of the nanolaminated transition metal carbide Ti2AlC has been investigated by bulk-sensitive soft x-ray emission spectroscopy. The measured Ti L, C K and Al L emission spectra are compared with calculated spectra using ab initio density-functional theory including dipole matrix elements. The detailed investigation of the electronic structure and chemical bonding provides increased understanding of the physical properties of this type of nanolaminates. Three different types of bond regions are identified; the relatively weak Ti 3d - Al 3p hybridization 1 eV below the Fermi level, and the Ti 3d - C 2p and Ti 3d - C 2s hybridizations which are stronger and deeper in energy are observed around 2.5 eV and 10 eV below the Fermi level, respectively. A strongly modified spectral shape of the 3s final states in comparison to pure Al is detected for the buried Al monolayers indirectly reflecting the Ti 3d - Al 3p hybridization. The differences between the electronic and crystal structures of Ti2AlC, Ti3AlC2 and TiC are discussed in relation to the number of Al layers per Ti layer in the two former systems and the corresponding change of the unusual materials properties.
The electronic structures of epitaxially grown films of Ti3AlC2, Ti3SiC2 and Ti3GeC2 have been investigated by bulk-sensitive soft X-ray emission spectroscopy. The measured high-resolution Ti L, C K, Al L, Si L and Ge M emission spectra are compared with ab initio density-functional theory including core-to-valence dipole matrix elements. A qualitative agreement between experiment and theory is obtained. A weak covalent Ti-Al bond is manifested by a pronounced shoulder in the Ti L-emission of Ti3AlC2. As Al is replaced with Si or Ge, the shoulder disappears. For the buried Al and Si-layers, strongly hybridized spectral shapes are detected in Ti3AlC2 and Ti3SiC2, respectively. As a result of relaxation of the crystal structure and the increased charge-transfer from Ti to C, the Ti-C bonding is strengthened. The differences between the electronic structures are discussed in relation to the bonding in the nanolaminates and the corresponding change of materials properties.
We study the crystalline and electronic properties of the $textrm{Fe}_{1-x}textrm{Co}_xtextrm{Se}$ system ($x=0$, 0.25, 0.5, 0.75, and 1.0) using X-ray diffraction, X-ray spectroscopy and density functional theory. We show that the introduction of Co $3d$ states in FeSe relaxes the bond strengths and induces a structural transition from tetragonal to hexagonal whose crossover takes place at $xapprox0.38$. This structural transition in turn modifies the magnetic order which can be related to the spin state. Using resonant inelastic X-ray spectroscopy we estimate the spin state of the system; FeSe is found to be in a high spin state (S=2), but Fe is reduced to a low spin state upon Co substitution of $x le 0.25$, well below the structural transition. Finally, we show evidence that FeSe is a moderately correlated system but the introduction of Co into the host lattice weakens the correlation strength for $xge0.25$. These novel findings are important to unravel the mechanisms responsible for the superconducting state in iron-chalcogenide superconductors.
In van der Waals heterostructures, the periodic potential from the Moire superlattice can be used as a control knob to modulate the electronic structure of the constituent materials. Here we present a nanoscale angle-resolved photoemission spectroscopy (Nano-ARPES) study of transferred graphene/h-BN heterostructures with two different stacking angles of 2.4{deg} and 4.3{deg} respectively. Our measurements reveal six replicas of graphene Dirac cones at the superlattice Brillouin zone (SBZ) centers. The size of the SBZ and its relative rotation angle to the graphene BZ are in good agreement with Moire superlattice period extracted from atomic force microscopy (AFM) measurements. Comparison to epitaxial graphene/h-BN with 0{deg} stacking angles suggests that the interaction between graphene and h-BN decreases with increasing stacking angle.
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