Surface- and strain-tuning of the optical dielectric function in epitaxially grown CaMnO3

Abstract

We report a strong thickness dependence of the complex frequency-dependent optical dielectric function ϵ̃(ω) over a spectral range from 1.24 to 5 eV in epitaxial CaMnO3(001) thin films on SrTiO3(001), LaAlO3(001), and SrLaAlO4(001). A doubling of the peak value of the imaginary part of ϵ̃(ω) and spectral shifts of 0.5 eV for a given magnitude of absorption are observed. On the basis of experimental analyses and first-principles density functional theory calculations, contributions from both surface states and epitaxial strain to the optical dielectric function of CaMnO3 are seen. Its evolution with thickness from 4 to 63 nm has several regimes. In the thinnest, strain-coherent films, the response is characterized by a significant contribution from the free surface that dominates strain effects. However, at intermediate and larger thicknesses approaching the bulk-like film, strain coherence and partial strain relaxation coexist and influence ϵ̃(ω).