L -gap surface resonance at Pt(111): Influence of atomic structure, d bands, and spin-orbit interaction

Abstract

Pt(111) hosts a surface resonance with peculiar properties concerning energy vs momentum dispersion and spin texture. At variance with the free-electron-like behavior of the L-gap Shockley-type surface states on the fcc(111) surfaces of Au, Ag, and Cu, it splits into several branches with distinct spin polarization around the center of the surface Brillouin zone Γ¯. Theoretical predictions based on density-functional theory vary depending on the particular functionals used. To clarify this issue, we investigate the atomic structure of Pt(111) by low-energy electron diffraction and the unoccupied electronic structure by spin- and angle-resolved inverse photoemission. The experimental results are backed by theoretical studies using different functionals, which show that the characteristics of the surface band depend critically on the lattice constant. From the analysis of the energy-dependent low-energy electron diffraction intensities, we derive structural parameters of the Pt(111) surface relaxation with high accuracy. In addition, we give an unambiguous definition of the nonequivalent mirror-plane directions Γ¯M¯ and Γ¯M¯′ at fcc(111) surfaces, which is consistent with band-structure calculations and inverse-photoemission data. Concerning the surface resonance at the bottom of the L gap, we identified a delicate interplay of several contributions. Lattice constant, hybridization with d bands, and the influence of spin-orbit interaction are critical ingredients for understanding the peculiar energy dispersion and spin character of the unoccupied surface resonance. Published by the American Physical Society 2024