Mott-Derived Local Moments and Kondo Hybridization in a d-electron Kagome lattice

Abstract

Unlike canonical Kondo lattices in f-electron systems, where localized f orbitalsnaturally provide local moments, d-electron Kondo lattices require a distinct mechanism for local-moment formation. However, the study of d-electron Kondo lattices in bulk materials remains far from settled, particularly with regard to the microscopic origin of the local moments. Here, we report a microscopic mechanism for this process in the bilayer kagome metal CsCr6Sb6, where strong correlations drive a Mott splitting of the kagome flat band to supply the requisite local moments. By combining STM/STS and ARPES, we resolve a spectroscopic hierarchy between high-energy correlation effects and low temperature hybridization. Low-temperature STS reveals a robust asymmetric suppression of the density of states near EF that is well captured phenomenologically by a Fano-type lineshape, while ARPES detects a sharp quasiparticlepeak near EF. These low-energy signatures evolveon the same temperature scale and disappear upon warming, consistent with the onset of Kondo hybridization. At the same time, STS resolves symmetric humps at approximately +-50 mV and ARPES identifies a weakly dispersive feature around 50 meV below EF; unlike the near-EF hybridization signatures, these features persist to substantially higher temperatures. This separation of energy and temperature scales supports a two-stage picture in which a kagome flat band first undergoes correlation-driven splitting into lower and upper Hubbard bands, and the occupied lower Hubbard band supplies the local moments that later hybridize with itinerant electrons at lower temperature. Our results therefore move beyond the phenomenology of a kagome Kondo lattice candidate and instead provide a microscopic spectroscopic picture linking Mottness to Kondo hybridization in a frustrated d-electron system.