The branching ratio of core-valence transitions in electron energy-loss spectroscopy and x-ray absorption spectroscopy is linearly related to the expectation value of the spin-orbit operator of the valence states. Here, we analyze the branching ratio of the edges in the actinides and find that the spin-orbit sum rule gives an accurate result without the need to include the core-valence interactions. The branching ratio is not only useful to study the variations in the spin-orbit interaction, it also allows us to constrain the count for given angular-momentum coupling conditions.
31 March 2001 in The Journal of Physical Chemistry B
We report the first application of valence-band photoemission to a quantum-dot system. Photoemission spectra of cadmium sulfide quantum dots, ranging in size from 12 to 35 Å radius, were obtained using photon energies of 20 to 70 eV. The spectra are qualitatively similar to those obtained for bulk cadmium sulfide, but show a shift in the valence-band maximum with size.
The surface electronic states of have been measured using spin- and angle-resolved photoemission. We directly demonstrate that the surface bands are both split and spin-polarized by the spin-orbit interaction in association with the loss of inversion symmetry near a surface. We observe 100% spin polarization of the surface states, with the spins aligned in the plane of the surface and oriented in a circular fashion relative to the symmetry point. In contrast, no measurable polarization of nearby bulk states is observed.
Angle-resolved photoemission extended fine structure from adsorbate core levels yields complete, accurate surface structures without resort to trial-and-error comparisons to theory. Scattering peaks from individual substrate atoms were observed with use of photoemission from and , along [011]. Fourfold-hollow site geometries were found for both systems, with interatomic distances of Å and Å.
Synchrotron-radiation-based x-ray absorption, electron energy-loss spectroscopy in a transmission electron microscope, multielectronic atomic spectral simulations, and improved first-principles calculations (generalized gradient approximation in the local density approximation) have been used to investigate the electronic structure of the light actinides: , , and . It will be shown that the spin-orbit interaction can be used as a measure of the degree of localization of valence electrons in a material. The spin-orbit interaction in the light actinide metals , , and , has been determined using the branching ratio of the white line peaks of the edges, which correspond to transitions. Examination of the branching ratios and spin-orbit interaction shows that the apparent spin-orbit splitting is partially quenched in , but is strongly dominant in . These results are fully quantified using the sum rule. This picture of the actinide electronic structure is confirmed by comparison with the results of electronic structure calculations for , , and , which in turn are supported by a previous bremsstrahlung isochromat spectroscopy experiment.
About Me
Staff Scientist/Principal Investigator, Lawrence Livermore Natl. Lab.,1989-2015
Staff Scientist/Principal Investigator, Lawrence Livermore Natl. Lab.,1989-2015