Correlated electronic structure and optical response of rare-earth-based semiconductors

Abstract

Simultaneous occurrence of the Mott and band gap in correlated semiconductors results in a complex optical response with the nature of the absorption edge difficult to resolve both experimentally and theoretically. Here, we combine a dynamical mean-field theory approach to localized 4f shells with an improved description of band gaps by a semi-local exchange-correlation potential to calculate the optical properties of the light rare-earth fluorosulfides LnSF (Ln=Pr, Nd, Sm, Gd) from first principles. In agreement with experiment, we find the absorption edge in SmSF to stem from S-3p to Sm-4f transitions, while the Gd compound behaves as an ordinary p-d gap semiconductor. In the unexplored PrSF and NdSF systems we predict a rather unique occurrence of strongly hybridized 4f-5d states at the bottom of the conduction band. The nature of the absorption edge underlies a peculiar anisotropy of the optical conductivity in each system.

References in corpus (4)

• Continuous-time Monte Carlo methods for quantum impurity models
• Dynamical Mean-Field Theory within an Augmented Plane-Wave Framework: Assessing Electronic Correlations in the Iron Pnictide LaFeAsO
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• Rare-Earth vs. Heavy Metal Pigments and their Colors from First Principles

Cited by in corpus (4)

• Electronic structure of rare-earth mononitrides: quasiatomic excitations and semiconducting bands
• A Theory for Colors of Strongly Correlated Electronic Systems
• Relation between crystal structure and optical properties in the correlated blue pigment YIn${}_{1-x}$Mn${}_x$O${}_3$
• Combining semi-local exchange with dynamical mean-field theory: electronic structure and optical response of rare-earth sesquioxides