Improved method for generating exchange-correlation potentials from electronic wave functions.

Ryabinkin, Kohut, and Staroverov (RKS) [Phys. Rev. Lett. 115, 083001 (2015)] devised an iterative method for reducing many-electron wave functions to Kohn-Sham exchange-correlation potentials, vXC(𝐫). For a given type of wave function, the RKS method is exact (Kohn-Sham-compliant) in the basis-set limit; in a finite basis set, it produces an approximation to the corresponding basis-set-limit vXC(𝐫). The original RKS procedure works very well for large basis sets but sometimes fails for commonly used (small and medium) sets. We derive a modification of the method's working equation that makes the RKS procedure robust for all Gaussian basis sets and increases the accuracy of the resulting exchange-correlation potentials with respect to the basis-set limit.