Applicability of density functional theory to model molecular solvation in superfluid 4He

Density functional theory (DFT) has been extensively applied to model solvation of atomic and molecular species ("impurities") in superfluid helium. The interaction between the impurity and the surrounding liquid may range from purely repulsive (e.g. alkali metal atoms and most diatomic excimers) to deeply bound potentials (e.g. aromatic compounds). In order to apply DFT to model processes relevant to low temperature chemistry in superfluid 4 He, it is essential to obtain the limits of applicability of the theory. For purely repulsive potentials, the spatial gradient of the liquid density remains small and DFT is expected to produce accurate results. This has been verified previously by comparing DFT results to quantum Monte Carlo calculations. For strong binding potentials, however, DFT fails since the individual He atoms tend to localize about the potential minimum. The present work tests the accuracy of DFT between the weakly and strongly bound regimes. This is done by comparing DFT and quantum Monte Carlo (diffusion Monte Carlo) results for various realistic model potentials with varying degree of binding.