Orbital-free density-functional theory (DFT) is in principle, at least, a linear-scaling quantum mechanical method with an ultra-low computational cost. Indeed, orbital-free DFT has already allowed for the quantum-mechanical treatment of periodic metallic systems with millions of atoms.<br/> <br/>The major challenge of orbital-free DFT is the development of accurate kinetic-energy functionals and the optimization of the density for a given number of electrons. We here address the optimization problem, presenting a robust second-order saddle-point method for the simultaneous optimization of the density and chemical potential of molecular electronic systems, providing fast and tight convergence even in difficult cases with poor starting guesses.

Robust all-electron optimization of orbital-free density-functional theory

2019 Fall National Meeting

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.