Electronic structure, properties, and phase stability of inorganic crystals: A pseudopotential plane-wave study

Recent developments in density functional theory (DFT) methods applicable to studies of large periodic systems are outlined. During the past three decades, DFT has become an essential part of computational materials science, addressing problems in materials design and processing. The theory allows us to interpret experimental data and to generate property data (such as binding energies of molecules on surfaces) for known materials, and also serves as an aid in the search for and design of novel materials and processes. A number of algorithmic implementations are currently being used, including ultrasoft pseudopotentials, efficient iterative schemes for solving the one-electron DFT equations, and computationally efficient codes for massively parallel computers. The first part of this article provides an overview of plane-wave pseudopotential DFT methods. Their capabilities are subsequently illustrated by examples including the prediction of crystal structures, the study of the compressibility of minerals, and applications to pressure-induced phase transitions. Future theoretical and computational developments are expected to lead to improved accuracy and to treatment of larger systems with a higher computational efficiency. © 2000 John Wiley & Sons, Inc. Int J Quant Chem 77: 895–910, 2000