Study of crystal-field splitting in ultrathin CePt$_5$ layers by Raman spectroscopy

Abstract

Low-temperature electronic properties of rare-earth intermetallics are substantially influenced by the symmetry and magnitude of the crystal electric field. The direct spectroscopic analysis of crystal field splitting can be challenging, especially in low-dimensional systems, because it requires both high spectral resolution and pronounced sensitivity. We demonstrate the eligibility of electronic Raman spectroscopy for this purpose by the direct determination of the $4f$ level splitting in ultra-thin ordered CePt$_5$ films down to 1.7 nm thickness on Pt(111). Crystal field excitations of Ce $4f$ electrons give rise to Raman peaks with energy shifts up to $\approx$ 25 meV. Three distinct peaks occur which we attribute to inequivalent Ce sites, located (i) at the interface to the substrate, (ii) next to the Pt-terminated surface, and (iii) in the CePt$_5$ layers in between. The well-resolved Raman signatures allow us to identify a reduced crystal field splitting at the interface and an enhancement at the surface, highlighting its strong dependence on the local atomic environment.