Unraveling the Impact of Graphene Addition to Thermoelectric SrTiO₃ and La-Doped SrTiO₃ Materials: A Density Functional Theory Study

We present a detailed theoretical investigation of the interaction of graphene with the SrO-terminated (001) surface of pristine and La-doped SrTiO₃. The adsorption of graphene is thermodynamically favorable with interfacial adsorption energies of −0.08 and −0.32 J/m² to pristine SrTiO₃ and La-doped SrTiO₃ surfaces, respectively. We find that graphene introduces C 2p states at the Fermi level, rendering the composite semimetallic, and thus the electrical properties are predicted to be highly sensitive to the amount and quality of the graphene. An investigation of the lattice dynamics predicts that graphene adsorption may lead to a 60–90% reduction in the thermal conductivity due to a reduction in the phonon group velocities, accounting for the reduced thermal conductivity of the composite materials observed experimentally. This effect is enhanced by La doping. We also find evidence that both La dopant ions and adsorbed graphene introduce low-frequency modes that may scatter heat-carrying acoustic phonons, and that, if present, these effects likely arise from stronger phonon–phonon interactions.