One-crossing Approximation Research Articles

Renormalization of spin excitations and Kondo effect in open-shell nanographenes

We study spin excitations and Kondo effect in open-shell nanographenes, motivated by recent scanning tunneling inelastic spectroscopy experiments. Specifically, we consider three systems, the triangulene, the extended triangulene with rocket shape, both with an $S=1$ ground state, and a triangulene dimer with $S=0$ on account of intermolecular exchange. We focus on the consequences of hybridization of the nanographene zero-modes with a conducting substrate on the $dI/dV$ lineshapes associated with spin excitations. The partially filled nanographene zero-modes coupled to the conduction electrons in the substrate constitute multi-orbital Anderson impurity models that we solve in the one-crossing approximation which treats the coupling to the substrate to infinite order. We find that the coupling to the substrate leads to (i) renormalization of the spin flip excitation energies of the bare molecule, (ii) broadening of the spectral features and (iii) the emergence of zero bias Kondo peaks for the $S=1$ ground states. The calculated substrate induced shift of the spin excitation energies is found to be significantly larger than their broadening, which implies that this effect has to be considered when comparing experimental results and theory.

Quantitative comparison of Anderson impurity solvers applied to transport in quantum dots

We study the single impurity Anderson model (SIAM) using the equations of motion method (EOM), the non-crossing approximation (NCA), the one-crossing approximation (OCA), and Wilson’s numerical renormalization group (NRG). We calculate the density of states and the linear conductance focusing on their dependence on the chemical potential and on the temperature paying special attention to the Kondo and Coulomb blockade regimes for a large range of model parameters. We report that some standard approximations based on the EOM technique display a rather unexpected poor behavior in the Coulomb blockade regime even at high temperatures. Our study offers a critical comparison between the different methods as well as a detailed compilation of the shortcomings and limitations due the approximations involved in each technique, thus allowing for a cost-benefit analysis of the different solvers that considers both numerical precision and computational performance.

Comparative study of nonequilibrium insulator-to-metal transitions in electron-phonon systems

We study equilibrium and nonequilibrium properties of electron-phonon systems described by the Hubbard-Holstein model using the dynamical mean-field theory. In equilibrium, we benchmark the results for impurity solvers based on the one-crossing approximation and slave-rotor approximation against non-perturbative numerical renormalization group reference data. We also examine how well the low energy properties of the electron-boson coupled systems can be reproduced by an effective static electron-electron interaction. The one-crossing and slave-rotor approximations are then used to simulate insulator-to-metal transitions induced by a sudden switch-on of the electron-phonon interaction. The slave-rotor results suggest the existence of a critical electron-phonon coupling above which the system is transiently trapped in a non-thermal metallic state with coherent quasiparticles. The same quench protocol in the one-crossing approximation results in a bad metallic state.

Orbital-dependent correlations in PuCoGa5

We investigate the normal state of the superconducting compound PuCoGa$_5$ using the combination of density functional theory (DFT) and dynamical mean field theory (DMFT), with the continuous time quantum Monte Carlo (CTQMC) and the vertex-corrected one-crossing approximation (OCA) as the impurity solvers. Our DFT+DMFT(CTQMC) calculations suggest a strong tendency of Pu-5$f$ orbitals to differentiate at low temperatures. The renormalized 5$f_{5/2}$ states exhibit a Fermi-liquid behavior whereas one electron in the 5$f_{7/2}$ states is at the edge of a Mott localization. We find that the orbital differentiation is manifested as the removing of 5$f_{7/2}$ spectral weight from the Fermi level relative to DFT. We corroborate these conclusions with DFT+DMFT(OCA) calculations which demonstrate that 5$f_{5/2}$ electrons have a much larger Kondo scale than the 5$f_{7/2}$.

DMFT Study for Valence Fluctuations in the Extended Periodic Anderson Model

We study valence fluctuations at finite temperatures in the extended periodic Anderson model, where the Coulomb interaction between conduction and localized f-electrons is taken into account, using dynamical mean-field theory combined with the continuous-time quantum Monte Carlo (CT-QMC) method. The valence transition with the hysteresis is clearly found, indicating the first-order phase transition between the Kondo and mixed-valence states. We demonstrate that spin correlation rapidly develops when the system approaches the valence transition point. The comparison of the impurity solvers, the CT-QMC, non-crossing approximation, and one-crossing approximation, is also addressed.

Reliability of the one-crossing approximation in describing the Mott transition

We assess the reliability of the one-crossing approximation (OCA) approach in a quantitative description of the Mott transition in the framework of the dynamical mean field theory (DMFT). The OCA approach has been applied in conjunction with DMFT to a number of heavy-fermion, actinide, transition metal compounds and nanoscale systems. However, several recent studies in the framework of impurity models pointed out serious deficiencies of OCA and raised questions regarding its reliability. Here we consider a single band Hubbard model on the Bethe lattice at finite temperatures and compare the results of OCA to those of a numerically exact quantum Monte Carlo (QMC) method. The temperature-local repulsion U phase diagram for the particle-hole symmetric case obtained by OCA is in good agreement with that of QMC, with the metal–insulator transition captured very well. We find, however, that the insulator to metal transition is shifted to higher values of U and, simultaneously, correlations in the metallic phase are significantly overestimated. This counter-intuitive behaviour is due to simultaneous underestimations of the Kondo scale in the metallic phase and the size of the insulating gap. We trace the underestimation of the insulating gap to that of the second moment of the high-frequency expansion of the impurity spectral density. Calculations of the system away from the particle-hole symmetric case are also presented and discussed.

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

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(0 0 1) 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.

Comparative DMFT study of theeg-orbital Hubbard model in thin films

Heterostructures of transition-metal oxides have emerged as a new route to engineer electronic systems with desired functionalities. Motivated by these developments, we study a two-orbital Hubbard model in a thin-film geometry confined along the cubic [001] direction using the dynamical mean-field theory. We contrast the results of two approximate impurity solvers (exact diagonalization and one-crossing approximation) to the results of the numerically exact continuous-time quantum Monte Carlo solver. Consistent with earlier studies, we find that the one-crossing approximation performs well in the insulating regime, while the advantage of the exact-diagonalization-based solver is more pronounced in the metallic regime. We then investigate various aspects of strongly correlated ${e}_{g}$-orbital systems in thin-film geometries. In particular, we show how the interfacial orbital polarization dies off quickly a few layers from the interface and how the film thickness affects the location of the interaction-driven Mott transition. In addition, we explore the changes in the electronic structure with varying carrier concentration and identify large variations of the orbital polarization in the strongly correlated regime.

Sum rule violation in self-consistent hybridization expansions

We show that for multi-orbital quantum impurity models the non-crossing approximation and one-crossing approximation versions of the self-consistent hybridization expansions violate the sum rules relating the coefficients of the high-frequency expansion of the self energy and the product of the self energy and Green function to thermodynamic expectation values. Comparison of non-crossing/one-crossing results to numerically exact quantum Monte-Carlo calculations shows that the consistency with sum rules provides a useful estimate of the reliability of the approximations. The sum rule violations are more pronounced, and therefore the quality of the non-crossing/one-crossing approximation is poorer, in situations with multiple orbitals and away from particle-hole symmetry but becomes less severe as the correlation strength increases. The one crossing approximation is markedly superior to the non-crossing approximation.

Effects of vertex corrections on diagrammatic approximations applied to the study of transport through a quantum dot

In the present work, we calculate the conductance through a single quantum dot weakly coupled to metallic contacts. We use the spin-1/2 Anderson model to describe the quantum dot, while considering a finite Coulomb repulsion. We solve the interacting system using the noncrossing approximation (NCA) and the one-crossing approximation (OCA). We obtain the linear response conductance as a function of temperature and energy position of the localized level. From the comparison of both approximations we extract the role of the vertex corrections, which are introduced in the OCA calculations and neglected in the NCA scheme. As a function of the energy position, we observe that the diagrams omitted within the NCA are really important for appropriately describing transport phenomena in Kondo systems as well as in the mixed valence regime. On the other hand, as a function of temperature, the corrections introduced by the OCA partly recover the universal scaling properties known from numerical approaches such as the numerical renormalization group.

Kondo Effect and Conductance of Nanocontacts with Magnetic Impurities

We study the impact of dynamical correlations on the electronic structure and coherent transport properties of Cu nanocontacts hosting a single magnetic impurity (Ni, Co, Fe) in the contact region. The strong dynamical correlations of the impurity 3d electrons are fully taken into account by combining density-functional calculations with a dynamical treatment of the impurity 3d shell in the one-crossing approximation. We find that dynamical correlations give rise to the Kondo effect and lead to Fano features in the coherent transport characteristics similar to those observed in related experiments.