Pier Paolo Baruselli

Kondo conductance across the smallest spin 1/2 radical molecule

Significance Molecular electronics, with molecules functioning as the basic building blocks of circuits, is considered by some to be one of the contenders for next-generation electronics. Radical molecules are interesting because a quantum phenomenon, the Kondo effect, involving the radical’s unpaired electron and its spin, has the potential to enhance and control conductance. Examples of molecular Kondo are known experimentally in geometries including mechanical break junctions and scanning tunneling spectroscopy (STS), but so far it has not been possible to make accurate theoretical predictions. Here we predict the Kondo effect expected for the simplest molecular radical, nitric oxide, on a gold surface. Subsequently we verify that experimentally by STS. Both agreements and discrepancies offer a quantitative lesson of considerable future use. Molecular contacts are generally poorly conducting because their energy levels tend to lie far from the Fermi energy of the metal contact, necessitating undesirably large gate and bias voltages in molecular electronics applications. Molecular radicals are an exception because their partly filled orbitals undergo Kondo screening, opening the way to electron passage even at zero bias. Whereas that phenomenon has been experimentally demonstrated for several complex organic radicals, quantitative theoretical predictions have not been attempted so far. It is therefore an open question whether and to what extent an ab initio-based theory is able to make accurate predictions for Kondo temperatures and conductance lineshapes. Choosing nitric oxide (NO) as a simple and exemplary spin 1/2 molecular radical, we present calculations based on a combination of density functional theory and numerical renormalization group (DFT+NRG), predicting a zero bias spectral anomaly with a Kondo temperature of 15 K for NO/Au(111). A scanning tunneling spectroscopy study is subsequently carried out to verify the prediction, and a striking zero bias Kondo anomaly is confirmed, still quite visible at liquid nitrogen temperatures. Comparison shows that the experimental Kondo temperature of about 43 K is larger than the theoretical one, whereas the inverted Fano lineshape implies a strong source of interference not included in the model. These discrepancies are not a surprise, providing in fact an instructive measure of the approximations used in the modeling, which supports and qualifies the viability of the density functional theory and numerical renormalization group approach to the prediction of conductance anomalies in larger molecular radicals.

Ferromagnetic Kondo Effect in a Triple Quantum Dot System

A simple device of three laterally coupled quantum dots, the central one contacted by metal leads, provides a realization of the ferromagnetic Kondo model, which is characterized by interesting properties like a nonanalytic inverted zero-bias anomaly and an extreme sensitivity to a magnetic field. Tuning the gate voltages of the lateral dots allows us to study the transition from a ferromagnetic to antiferromagnetic Kondo effect, a simple case of a Berezinskii-Kosterlitz-Thouless transition. We model the device by three coupled Anderson impurities that we study by numerical renormalization group. We calculate the single-particle spectral function of the central dot, which at zero frequency is proportional to the zero-bias conductance, across the transition, both in the absence and in the presence of a magnetic field.

Metallic, magnetic and molecular nanocontacts

Scanning tunnelling microscopy and break-junction experiments realize metallic and molecular nanocontacts that act as ideal one-dimensional channels between macroscopic electrodes. Emergent nanoscale phenomena typical of these systems encompass structural, mechanical, electronic, transport, and magnetic properties. This Review focuses on the theoretical explanation of some of these properties obtained with the help of first-principles methods. By tracing parallel theoretical and experimental developments from the discovery of nanowire formation and conductance quantization in gold nanowires to recent observations of emergent magnetism and Kondo correlations, we exemplify the main concepts and ingredients needed to bring together ab initio calculations and physical observations. It can be anticipated that diode, sensor, spin-valve and spin-filter functionalities relevant for spintronics and molecular electronics applications will benefit from the physical understanding thus obtained.

Co adatoms on Cu surfaces: ballistic conductance and Kondo temperature

The Kondo zero bias anomaly of Co adatoms probed by scanning tunneling microscopy is known to depend on the height of the tip above the surface, and this dependence is different on different low index Cu surfaces. On the (100) surface, the Kondo temperature first decreases then increases as the tip approaches the adatom, while on the (111) surface it is virtually unaffected. These trends are captured by combined density functional theory and numerical renormalization group (DFT+NRG) calculations. The adatoms are found to be described by an S = 1 Anderson model on both surfaces, and ab initio calculations help identify the symmetry of the active d orbitals. We correctly reproduce the Fano lineshape of the zero bias anomaly for Co/Cu(100) in the tunneling regime but not in the contact regime, where it is probably dependent on the details of the tip and contact geometry. The lineshape for Co/Cu(111) is presumably affected by the presence of surface states, which are not included in our method. We also discuss the role of symmetry, which is preserved in our model scattering geometry but most likely broken in experimental conditions.

Distinct Topological Crystalline Phases in Models for the Strongly Correlated Topological Insulator SmB_{6}.

SmB_{6} was recently proposed to be both a strong topological insulator and a topological crystalline insulator. For this and related cubic topological Kondo insulators, we prove the existence of four different topological phases, distinguished by the sign of mirror Chern numbers. We characterize these phases in terms of simple observables, and we provide concrete tight-binding models for each phase. Based on theoretical and experimental results for SmB_{6} we conclude that it realizes the phase with C_{k_{z}=0}^{+}=+2, C_{k_{z}=π}^{+}=+1, C_{k_{x}=k_{y}}^{+}=-1, and we propose a corresponding minimal model.

Scanning tunneling spectroscopy and surface quasiparticle interference in models for the strongly correlated topological insulatorsSmB6andPuB6

SmB6 is one of the candidate compounds for topological Kondo insulators, a class of materials which combines a non-trivial topological band structure with strong electronic correlations. Here we employ a multiband tight-binding description, supplemented by a slave-particle approach to account for strong interactions, to theoretically study the surface-state signatures in scanning tunneling spectroscopy (STS) and quasiparticle interference (QPI). We discuss the spin structure of the three surface Dirac cones of SmB6 and provide concrete predictions for the energy and momentum dependence of the resulting QPI signal. Our results also apply to PuB6, a strongly correlated topological insulator with a very similar electronic structure.

Kondo holes in topological Kondo insulators: Spectral properties and surface quasiparticle interference

A fascinating type of symmetry-protected topological states of matter are topological Kondo insulators, where insulating behavior arises from Kondo screening of localized moments via conduction electrons, and non-trivial topology emerges from the structure of the hybridization between the local-moment and conduction bands. Here we study the physics of Kondo holes, i.e., missing local moments, in three-dimensional topological Kondo insulators, using a self-consistent real-space mean-field theory. Such Kondo holes quite generically induce in-gap states which, for Kondo holes at or near the surface, hybridize with the topological surface state. In particular, we study the surface-state quasiparticle interference (QPI) induced by a dilute concentration of surface Kondo holes and compare this to QPI from conventional potential scatterers. We treat both strong and weak topological-insulator phases and, for the latter, specifically discuss the contributions to QPI from inter-Dirac-cone scattering.

Kondo effect of magnetic impurities in nanotubes.

Transition metal impurities will yield zero bias anomalies in the conductance of well contacted metallic carbon nanotubes, but Kondo temperatures and geometry dependences have not been anticipated so far. Applying the density functional plus numerical renormalization group approach of Lucignano et al. to Co and Fe impurities in (4,4) and (8,8) nanotubes, we discover a huge difference of behaviour between outside versus inside adsorption of the impurity. The predicted Kondo temperatures and zero bias anomalies, tiny outside the nanotube, turn large and strongly radius dependent inside, owing to a change of symmetry of the magnetic orbital. Observation of this Kondo effect should open the way to a host of future experiments.

Magnetic impurities in nanotubes: From density functional theory to Kondo many-body effects

P. P. Baruselli, 2, 3 M. Fabrizio, 2 A. Smogunov, 5 R. Requist, and E. Tosatti 2, 6 SISSA, Via Bonomea 265, Trieste 34136, Italy CNR-IOM, Democritos Unitá di Trieste, Via Bonomea 265, Trieste 34136, Italy Institut für Theoretische Physik, Technische Universität Dresden, 01062 Dresden, Germany Voronezh State University, University Square 1, Voronezh 394006, Russia CEA, IRAMIS, SPCSI, F-91191 Gif-sur-Yvette Cedex, France ICTP, Strada Costiera 11, Trieste 34014, Italy (Dated: January 8, 2014)

Spin textures on general surfaces of the correlated topological insulatorSmB6

Employing the