Converge towards an exact electronic quantum many-body treatment of Kondo correlation in magnetic impurities with Full-cell DMFT

The Kondo effect is a prototypical quantum phenomenon arising from the interaction between localized electrons in a magnetic impurity and itinerant electrons in a metallic host. Although it has served as the testing ground for quantum many-body methods for decades, the precise description of Kondo physics with material specificity remains challenging. Here, we present a systematic ab initio dynamical mean-field theory (DMFT) approach to converge towards an exact zero-temperature electronic treatment of Kondo correlations. Our full-cell formulation of DMFT avoids deriving a low-energy model and has shown to overcome the associated orbital dependency on the infinite layer nickelate. The remaining approximations in the embedding theory are systematically improvable, and here we further attempt to quantify and converge those errors. Across a series of 3d transition metals, we extract Kondo temperatures matching the subtle experimental trends, with an accuracy far exceeding that of standard models. We further obtain microscopic insight into the origin of these trends. More broadly, we demonstrate the possibility to start from fully ab initio many-body simulations and push towards the realm of converged predictions.