Evolution of ultra-flat band in van der Waals kagome semiconductor Pd3P2(S1-xSex)8

TL;DR

This study explores how selenium doping affects the structural, optical, and electronic properties of Pd3P2S8, revealing the evolution of flat bands and interlayer interactions in this van der Waals kagome semiconductor.

Contribution

It demonstrates the doping-induced modulation of flat bands and interlayer coupling, providing insights into the electronic structure evolution in 2D kagome materials.

Findings

Se doping decreases bandgap and expands unit cell

Interlayer hopping enhances with Se doping, strengthening interlayer coupling

Ultra-flat bands form in monolayers due to vanishing interlayer hopping

Abstract

We investigate the evolutions of structural parameters, optical properties, and electronic structures of van der Waals kagome semiconductor Pd3P2S8 with Se doping. When the doping level of Se increases, the bandgaps of Pd3P2(S1-xSex)8 single crystals decrease gradually, accompanying with the expanded unit cells. The first-principles calculations show that there is a flat band (FB) near the Fermi level in bulk Pd3P2S8. This FB mainly originates from the dz2-like orbitals of Pd atoms in the Pd kagome lattice, which has a finite interlayer electron hopping perpendicular to the PdS4 square plane. The interlayer hopping can be reinforced with the Se doping, inducing a stronger interlayer coupling via the chalcogen atoms at apical sites, which reduces the bandgap and enhances the cleavage energy. In contrast, the vanishing interlayer hopping in the two-dimensional limit results in the formation of ultra-FB in the monolayers of these compounds. The easy exfoliation and the existence of unique ultra-FB near EF make Pd3P2(S1-xSex)8 a model system to explore the exotic physics of FB in two-dimensional kagome lattice.