Insights into the spurious long-range nature of local rs-dependent non-local exchange-correlation kernels

A systematic route to go beyond the exact exchange plus random phase approximation ( RPA) is to include a physical exchange-correlation kernel in the adiabatic-connection fluctuation-dissipation theorem. In the previous study [ D. Lu, J. Chem. Phys. 140, 18A520 ( 2014)], we found that nonlocal kernels with a screening length depending on the local Wigner-Seitz radius, r(s)(r), suffer an error associated with a spurious long-range repulsion in van der Waals bounded systems, which deteriorates the binding energy curve as compared to RPA. We analyze the source of the error and propose to replace r(s)(r) by a global, average r(s) in the kernel. Exemplary studies with the Corradini, del Sole, Onida, and Palummo kernel show that while this change does not affect the already outstanding performance in crystalline solids, using an average r(s) significantly reduces the spurious long-range tail in the exchange-correlation kernel in van der Waals bounded systems. When this method is combined with further corrections using local dielectric response theory, the binding energy of the Kr dimer is improved three times as compared to RPA. Published by AIP Publishing.