14 and 15 for overviews) and capable of very high accuracy, but the development and computational costs are severe. Post-HF technology is well developed (see, e.g., Refs. Thus post-HF methods, adding to Hartree-Fock numerous other determinants involving excited or “virtual” orbitals, are generally required for viable chemical computations. Some molecules, F 2, for example, are not even bound at the Hartree-Fock level. Bond energies are significantly underestimated. HF theory, while immensely more useful than TFD, is still not accurate enough for energy predictions in chemistry. This Perspective outlines the history, basic concepts, and present status of KS-DFT in chemical physics, and offers suggestions for its future development. I am hopeful the Kohn-Sham philosophical, theoretical, and computational framework can be preserved. If we are not mindful, however, these pressures may submerge the theory in the wave-function sea. Today KS-DFT finds itself under increasing pressure to deliver higher and higher accuracy and to adapt to ever more challenging problems. The rise of KS-DFT in chemical physics began in earnest in the mid 1980s, when crucial developments in its exchange-correlation term gave the theory predictive power competitive with well-developed wave-function methods. Its popularity stems from its beautifully simple conceptual framework and computational elegance.

Since its formal inception in 1964–1965, Kohn-Sham density-functional theory (KS-DFT) has become the most popular electronic structure method in computational physics and chemistry.

Amsterdam density functional .21 files