The recent focus on topological insulators is due to the scientific interest in the new state of quantum matter as well as the technology potential for a new generation of THz optoelectronics, ...spintronics and quantum computations. It is important to elucidate the dynamics of the Dirac fermions in the topologically protected surface state. Hence we utilized a novel ultrafast optical pump mid-infrared probe to explore the dynamics of Dirac fermions near the Dirac point. The femtosecond snapshots of the relaxation process were revealed by the ultrafast optics. Specifically, the Dirac fermion-phonon coupling strength in the Dirac cone was found to increase from 0.08 to 0.19 while Dirac fermions were away from the Dirac point into higher energy states. Further, the energy-resolved transient reflectivity spectra disclosed the energy loss rate of Dirac fermions at room temperature was about 1 meV/ps. These results are crucial to the design of Dirac fermion devices.
•Efficiency and limits of polarization dependent HAXPES for solid state systems.•The polarization dependence is less than expected from atomic cross-sections.•Still high contrast (∼20–25) for s ...orbitals.•Quantitative determination of contributions to the valence band.
We have investigated the efficiency and limits of polarization dependent hard X-ray photoelectron spectroscopy (HAXPES) in order to establish how well this method can be used to unravel quantitatively the contributions of the orbitals forming the valence band of solids. By rotating the energy analyzer rather than the polarization vector of the light using a phase retarder, we obtained the advantage that the full polarization of the light is available for the investigation. Using NiO, ZnO, and Cu2O as examples for solid state materials, we established that the polarization dependence is much larger than in photoemission experiments utilizing ultra-violet or soft X-ray light. Yet we also have discovered that the polarization dependence is less than complete on the basis of atomic calculations, strongly suggesting that the trajectories of the outgoing electrons are affected by appreciable side-scattering processes even at these high kinetic energies. We have found in our experiment that these can be effectively described as a directional spread of ±18° of the photoelectrons. This knowledge allows us to identify, for example, reliably the Ni 3d spectral weight of the NiO valence band and at the same time to demonstrate the importance of the Ni 4s for the chemical stability of the compound.
We report on our investigation of the electronic structure ofTi2O3using (hard) x-ray photoelectron and soft x-ray absorption spectroscopy. From the distinct satellite structures in the spectra, we ...have been able to establish unambiguously that the Ti-Tic-axis dimer in the corundum crystal structure is electronically present and forms ana1ga1gmolecular singlet in the low-temperature insulating phase. Upon heating, we observe a considerable spectral weight transfer to lower energies with orbital reconstruction. The insulator-metal transition may be viewed as a transition from a solid of isolated Ti-Ti molecules into a solid of electronically partially broken dimers, where the Ti ions acquire additional hopping in thea−bplane via theegπchannel, the opening of which requires consideration of the multiplet structure of the on-site Coulomb interaction.
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•Bulk-sensitive HAXPES study of 4f occupancy in Kondo semiconducting compounds.•Combination of configuration interaction model and full multiplet calculations.•Accurate correction of plasmon ...excitations in the core-level photoemission spectra.•Existence of substantial Kondo screening in magnetically ordered systems.
The occupancy of the 4fn contributions in the Kondo semiconductors CeM2Al10 (M=Ru, Os and Fe) has been quantitatively determined by means of bulk-sensitive hard X-ray photoelectron spectroscopy (HAXPES) on the Ce 3d core levels. Combining a configuration interaction scheme with full multiplet calculations allowed to accurately describe the HAXPES data despite the presence of strong plasmon excitations in the spectra. The configuration interaction parameters obtained from this analysis – in particular the hybridization strength Veff and the effective f binding energy Δf – indicate a slightly stronger exchange interaction in CeOs2Al10 compared to CeRu2Al10, and a significant increase in CeFe2Al10. This shows the existence of a substantial amount of Kondo screening in these magnetically ordered systems and places the entire CeM2Al10 family in the region of strong exchange interactions.
•Bulk-sensitive valence determination in CeMIn5 via HAXPES and quantitative analysis.•Comparison to other Ce systems of various hybridization strengths.•Identical f-occupation in CeMIn5 compounds ...confirmed by L-edge PFY-XAS.•Conclusion: transition elements act as perturbation only.•Crystal-field wave function may have important impact on ground state formation.
We present bulk-sensitive hard X-ray photoelectron spectroscopy (HAXPES) data of the Ce3d core levels and lifetime-reduced L-edge X-ray absorption spectroscopy (XAS) in the partial fluorescence yield (PFY) mode of the CeMIn5 family with M=Co, Rh, and Ir. The HAXPES data are analyzed quantitatively with a combination of full multiplet and configuration interaction model which allows correcting for the strong plasmons in the CeMIn5 HAXPES data, and reliable weights wn of the different fn contributions in the ground state are determined. The CeMIn5 results are compared to HAXPES data of other heavy fermion compounds and a systematic decrease of the hybridization strength Veff from CePd3 to CeRh3B2 to CeRu2Si2 is observed, while it is smallest for the three CeMIn5 compounds. The f-occupation, however, increases in the same sequence and is close to one for the CeMIn5 family. The PFY-XAS data confirm an identical f-occupation in the three CeMIn5 compounds and a phenomenological fit to these PFY-XAS data combined with a configuration interaction model yields consistent results.
Bulk sensitive hard x-ray photoelectron spectroscopy data of the Ce 3p core level of CeRu4Sn6 are presented. Using a combination of full multiplet and configuration iteration model we were able to ...obtain an accurate lineshape analysis of the data, thereby taking into account correlations for the strong plasmon intensities. We conclude that CeRu4Sn6 is a moderately mixed valence compound with a weight of 8% for the Ce f0 configuration in the ground state.
We report on a detailed experimental and theoretical study of the electronic structure of NiO. The charge-transfer nature of the band gap as well as the intricate interplay between local electronic ...correlations and band formation makes NiO to be a challenging case for a quantitative ab-initio modeling of its electronic structure. To reproduce the compensated-spin character of the first ionization state and the state created by hole doping requires a reliable determination of the charge transfer energy Δ relative to the Hubbard
U
. Furthermore, the presence of non-local screening processes makes it necessary to go beyond single-site many body approaches to explain the valence band spectrum.
Graphene and its bilayer are two-dimensional systems predicted to show exciting many-body effects near the neutrality point. The ideal tool to investigate spectrum reconstruction effects is ...angle-resolved photoemission spectroscopy (ARPES) as it probes directly the band structure with information about both energy and momentum. Here we reveal, by studying undoped exfoliated bilayer graphene with ARPES, two essential aspects of its many-body physics: the electron-phonon scattering rate has an anisotropic k-dependence and the type of electronic liquid is non-Fermi liquid. The latter behavior is evident from an observed electron-electron scattering rate that scales linearly with energy from 100 meV to 600 meV and that is associated with the proximity of bilayer graphene to a two-dimensional quantum critical point of competing orders.