Point defects have a strong impact on the performance of semiconductor and insulator materials used in technological applications, spanning microelectronics to energy conversion and storage. The nature of the dominant defect types, how they vary with processing conditions, and their impact on materials properties are central aspects that determine the performance of a material in a certain application. This information is, however, difficult to access directly from experimental measurements. Consequently, computational methods, based on electronic density functional theory (DFT), have found widespread use in the calculation of point-defect properties. Here we have developed the Python Charged Defect Toolkit (PyCDT) to expedite the setup and post-processing of defect calculations with widely used DFT software. PyCDT has a user-friendly command-line interface and provides a direct interface with the Materials Project database. This allows for setting up many charged defect calculations for any material of interest, as well as post-processing and applying state-of-the-art electrostatic correction terms. Our paper serves as a documentation for PyCDT, and demonstrates its use in an application to the well-studied GaAs compound semiconductor. We anticipate that the PyCDT code will be useful as a framework for undertaking readily reproducible calculations of charged point-defect properties, and that it will provide a foundation for automated, high-throughput calculations.

A π-electronic tight-binding (TB) model with, at most, three independent parameters is found to well fit the density functional theory results about the dispersions of the conduction and valence bands of α-, β-, γ -and (6,6,12)-graphyne. By means of such a toy model, the electron-hole symmetry in these graphynes is demonstrated. An explicit expression of the dispersion relation of α-graphyne is obtained. The position of the Dirac point on a particular -M line in the Brillouin zone of β-graphyne is analytically determined. The absence of Dirac cones in γ -graphyne is intuitively explained. Based on these interesting results, it is believed that this TB model provides a simple but effective theoretical approach for further study of the electronic and transport properties of these typical graphynes.

Bournonite (CuPbSbS) is an earth-abundant mineral with potential thermoelectric applications. This material has a complex crystal structure (space group Pmn2 #31) and has previously been measured to exhibit a very low thermal conductivity (κ < 1 W m K at T ≥ 300 K). In this study, we employ high-throughput density functional theory calculations to investigate how the properties of the bournonite crystal structure change with elemental substitutions. Specifically, we compute the stability and electronic properties of 320 structures generated via substitutions {Na-K-Cu-Ag}{Si-Ge-Sn-Pb}{N-P-As-Sb-Bi}{O-S-Se-Te} in the ABCD formula. We perform two types of transport calculations: the BoltzTraP model, which has been extensively tested, and a newer AMSET model that we have developed and which incorporates scattering effects. We discuss the differences in the model results, finding qualitative agreement except in the case of degenerate bands. Based on our calculations, we identify p-type CuPbSbSe, CuSnSbSe and CuPbAsSe as potentially promising materials for further investigation. We additionally calculate the defect properties, finding that n-type behavior in bournonite and the selected materials is highly unlikely, and p-type behavior might be enhanced by employing Sb-poor synthesis conditions to prevent the formation of Sb defects. Finally, we discuss the origins of various trends with chemical substitution, including the possible role of stereochemically active lone pair effects in stabilizing the bournonite structure and the effect of cation and anion selection on the calculated band gap.