Abstract

Density-functional theory has become one of the most powerful tools in the hands of the scientific community to understand, predict, or design the properties of novel materials and devices, notwithstanding the open challenges remaining in our quest towards predictive accuracy, and in our ability to perform simulations under realistic conditions.

Several of these challenges stem from the remnants of self-interaction in our electronic-structure framework, leading to qualitative failures in describing some of the fundamental processes involved in energy applications – from charge-transfer excitations to catalytic reactions to photoemission.

I will discuss these challenges in realistic case studies while suggesting possible solutions based on constrained DFT , on extended Hubbard functionals, or on imposing a generalized Koopmans’ theorem to DFT .