Towards a full ab initio theory of strong electronic correlations in nanoscale devices

Abstract

In this paper I give a detailed account of an ab initio methodology for describing strong electronic correlations in nanoscale devices hosting transition metal atoms with open $d$- or $f$-shells. The method combines Kohn-Sham Density Functional Theory for treating the weakly interacting electrons on a static mean-field level with non-perturbative many-body methods for the strongly interacting electrons in the open $d$- and $f$-shells. An effective description of the strongly interacting electrons in terms of a multi-orbital Anderson impurity model is obtained by projection onto the strongly correlated subspace properly taking into account the non-orthogonality of the atomic basis set. A special focus lies on the ab initio calculation of the effective screened interaction matrix U for the Anderson model. Solution of the effective Anderson model with the One-Crossing approximation or other impurity solver techniques yields the dynamic correlations within the strongly correlated subspace giving rise e.g. to the Kondo effect. As an example the method is applied to the case of a Co adatom on the Cu(001) surface. The calculated low-bias tunnel spectra show Fano-Kondo lineshapes similar to those measured in experiments. The exact shape of the Fano-Kondo feature as well as its width depend quite strongly on the filling of the Co $3d$-shell. Although this somewhat hampers accurate quantitative predictions regarding lineshapes and Kondo temperatures, the overall physical situation can be predicted quite reliably.

30 pages, 6 figures

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Cited by in corpus (13)

• Kondo resonance of a Co atom exchange coupled to a ferromagnetic tip
• Realistic theory of electronic correlations in nanoscopic systems
• Designing a mechanically driven spin-crossover molecular switch via organic embedding
• Dynamical Mean-Field Theory for spin-dependent electron transport in spin-valve devices
• The DFT+${\Sigma }_2$ method for electron correlation effects at transition metal surfaces
• Quantitative comparison of Anderson impurity solvers applied to transport in quantum dots
• Kondo physics of the Anderson impurity model by Distributional Exact Diagonalization
• Smart local orbitals for efficient calculations within density functional theory and beyond
• Interpreting Ultrafast Electron Transfer on Surfaces with a Converged First-Principles Newns-Anderson Chemisorption Function
• The interplay between strong correlation and adsorption distances
• Spin-orbit coupling and Kondo resonance in Co adatom on Cu(100) surface: DFT+ED study
• Plane-wave many-body corrections to the conductance in bulk tunnel junctions
• Transport properties of Co in Cu(100) from first principles