Structure and electronic properties of lead-free KTa1−xNbxO3: Accurate Wu–Cohen and screened-exchange study

We present first-principles calculations of structure and electronic properties of lead-free potassium tantalate niobate KTa1−xNbxO3 (KTN) using both Wu–Cohen functional (WC) and screened-exchange local density approximation (sX-LDA). WC predicts more accurate the lattice constants and atomic structure of KTN over standard LDA and generalized gradient approximation (GGA-PBE). sX-LDA successfully corrects the band-gap problem of LDA and PBE. The correctness of sX-LDA is further supported by excellent accordance between calculated absorption spectra and experiment. We show that in paraelectric state Ta and Nb atoms have obvious off-center displacements, which agree with experimental results and suggest that KTN are not displacive but order–disorder materials. We found that Ta and Nb have little contribution to valance band-top states, and therefore optical properties of KTN are not sensitive to Ta/Nb disorder.

► First-principles calculations of lead-free KTa1−xNbxO3 by Wu–Cohen and sX-LDA method. ► sX-LDA successfully corrects the band-gap problem of LDA and PBE. ► Obvious off-center displacements of Ta/Nb mean paraelectric KTN are order–disorder. ► Optical properties of KTN are not sensitive to Ta/Nb disorder.