  We present a method to make highly accurate pseudopotentials for use with
orbital-free density functional theory (OF-DFT) with given exchange-correlation
and kinetic energy functionals, which avoids the compounding of errors of
Kohn-Sham DFT and OF-DFT. The pseudopotentials are fitted to reference
(experimental or highly accurate quantum chemistry) values of interaction
energies, geometries, and mechanical properties, using a genetic algorithm.
This can enable routine large-scale ab initio simulations of many practically
relevant materials. Pseudopotentials for Li, Na, and Mg resulting in accurate
geometries and energies of different phases as well as of vacancy formation and
bulk moduli are presented as examples.
