Mapping of electron-hole excitations in the charge-density-wave system 1T-TiSe2 using resonant inelastic x-ray scattering.

In high-resolution resonant inelastic x-ray scattering at the Ti L edge of the charge-density-wave system 1T-TiSe(2), we observe sharp low energy loss peaks from electron-hole pair excitations developing at low temperature. These excitations are strongly dispersing as a function of the transferred momentum of light. We show that the unoccupied bands close to the Fermi level can effectively be probed in this broadband material. Furthermore, we extract the order parameter of the charge-density-wave phase from temperature-dependent measurements.

Evidence for an excitonic insulator phase in 1T-TiSe2.

We present a new high-resolution angle-resolved photoemission study of 1T-TiSe2 in both its room-temperature, normal phase and its low-temperature, charge-density wave phase. At low temperature the photoemission spectra are strongly modified, with large band renormalizations at high-symmetry points of the Brillouin zone and a very large transfer of spectral weight to backfolded bands. A calculation of the theoretical spectral function for an excitonic insulator phase reproduces the experimental features with very good agreement. This gives strong evidence in favor of the excitonic insulator scenario as a driving force for the charge-density wave transition in 1T-TiSe2.

Photoemission of a quantum cavity with a nonmagnetic spin separator.

Quantum well states are a consequence of confinement in a quantum cavity. In this study we investigate with photoemission the influence of the interface electronic structure on the quantum well state energy dispersion in ultrathin Mg(0001) films on W(110). Coupling between the sp-derived quantum well states and the substrate across the interface becomes manifest in a deviation from free electronlike dispersion behavior. Most importantly, we observe a marked level splitting, which is interpreted as due to the Rashba effect at the interface. Such an interfacial electron beam splitting on materials with strong spin-orbit coupling is an essential ingredient for novel spintronic devices. The combination of a quantum cavity with a heavy, electron reflecting substrate reveals spin-splitting effects in ultrathin films without conventional magnetism being involved.

Alloy formation of supported gold nanoparticles at their transition from clusters to solids: does size matter?

Gold nanoclusters of a size approaching the molecular limit (<3 nm) were prepared on Si substrates in order to study alloy formation on the nanometer scale. For this purpose, indium atoms are deposited on top of the gold particles at room temperature and the formation of AuIn(2) is studied by x-ray photoelectron spectroscopy in situ. It is observed that the alloy formation takes place independent of whether the particles electronically are in an insulating molecular or in a metallic state. Most important, however, closed packed full-shell clusters containing 55 Au atoms are found to exhibit an outstanding stability against alloying despite a large negative heat of formation of the bulk Au-In system. Thus, Au(55) clusters may play a significant role in the design of nanoscaled devices where chemical inertness is of crucial importance.

Oxidation-resistant gold-55 clusters.

Gold nanoparticles ranging in diameter from 1 to 8 nanometers were prepared on top of silicon wafers in order to study the size dependence of their oxidation behavior when exposed to atomic oxygen. X-ray photoelectron spectroscopy showed a maximum oxidation resistance for "magic-number" clusters containing 55 gold atoms. This inertness is not related to electron confinement leading to a size-induced metal-to-insulator transition, but rather seems to be linked to the closed-shell structure of such magic clusters. The result additionally suggests that gold-55 clusters may act as especially effective oxidation catalysts, such as for oxidizing carbon monoxide.

Chemically induced metal-to-insulator transition in Au55 clusters: effect of stabilizing ligands on the electronic properties of nanoparticles.

The cluster compound Au55(PPh3)12Cl6 has been reanalyzed by photoelectron spectroscopy giving direct evidence for a nonmetallic behavior of the individual Au clusters as long as their ligand shell remains intact. The exposure to x-rays during the measurements is found to partly decompose the shell by removal of the chlorine atoms, resulting in a metallic behavior of the clusters as demonstrated by a steplike intensity at the Fermi energy. These observations resolve a long-standing controversy about the metallic behavior of ligated Au clusters emphasizing, in addition, the influence of the local environment on the electronic properties of nanoscaled materials.