Structural and electronic properties of an azamacrocycle, C26H18N6

We compute the structure of an azamacrocycle, C26H18N6. Two approximatively planar elliptical structures with C2 or CI symmetry are found to be nearly degenerate. The roughly circular conformation observed in metal complexes turns out to be ~ 0.6 eV higher in energy. We suggest that this difference is mainly due to electrostatic interactions. We discuss the results on various levels of theory (Hartree-Fock, local density and gradient corrected density functional calculations).Comment: to appear in J Phys Chem

Fermi surface and heavy masses for UPd2_2Al3_3

We calculate the Fermi surface and the anisotropic heavy masses of UPd2Al3 by keeping two of the 5f electrons as localized. Good agreement with experiments is found. The theory contains essentially no adjustable parameter except for a small shift of the position of the Fermi energy of the order of a few meV. A discussion is given why localization of two f electrons is justified.Comment: 4 pages, 2 figure

Moment screening in the correlated Kondo lattice model

The magnetic correlations, local moments and the susceptibility in the correlated 2D Kondo lattice model at half filling are investigated. We calculate their systematic dependence on the control parameters J_K/t and U/t. An unbiased and reliable exact diagonalization (ED) approach for ground state properties as well as the finite temperature Lanczos method (FTLM) for specific heat and the uniform susceptibility are employed for small tiles on the square lattice. They lead to two major results: Firstly we show that the screened local moment exhibits non-monotonic behavior as a function of U for weak Kondo coupling J_K. Secondly the temperature dependence of the susceptibility obtained from FTLM allows to extract the dependence of the characteristic Kondo temperature scale T* on the correlation strength U. A monotonic increase of T* for small U is found resolving the ambiguity from earlier investigations. In the large U limit the model is equivalent to the 2D Kondo necklace model with two types of localized spins. In this limit the numerical results can be compared to those of the analytical bond operator method in mean field treatment and excellent agreement for the total paramagnetic moment is found, supporting the reliability of both methods.Comment: 19 pages, 9 figure

Superconductivity in heavy fermion compounds

We review the current state of experimental and theoretical investigations of heavy fermion superconductors. We discuss most of the Ce-based compounds like Ce122, Ce115, Ce218 and Ce131 classes and U-based superconductors like UBe_13 and UPd_2Al_3. In the former the emphasis is on the connection to quantum critical phenomena and non-Fermi liquid behaviour. Recent neutron scattering and hydrostatic pressure results on SDW/SC competition in the Ce122 system are included. For the U-compounds we discuss the significance of dual models with both localised and itinerant 5f electrons for mass enhancement and superconducting pair formation. Itinerant spin fluctuation theories for unconventional superconductivity are also reviewed.Comment: 74 pages, 29 figures. For a version of the manuscript including higher-resolution figures, see http://www.cpfs.mpg.de/~thalm/SCMaterials.pd

Approximative treatment of 5f-systems with partial localization due to intra-atomic correlations

Increasing experimental and theoretical evidence points towards a dual nature of the 5$f$ electrons in actinide-based strongly correlated metallic compounds, with some 5$f$ electrons being localized and others delocalized. In a recent paper (PRB xxx, 2004), we suggested the interplay of intra-atomic correlations as described by Hund's rules and a weakly anisotropic hopping (hybridization) as a possible mechanism. The purpose of the present work is to provide a first step towards a microscopic description of partial localization in solids by analyzing how well various approximation schemes perform when applied to small clusters. It is found that many aspects of partial localization are described appropriately both by a variational wavefunction of Gutzwiller type and by a treatment which keeps only those interactions which are present in LDA+U calculations. In contrast, the energies and phase diagram calculated within the Hartree Fock approximation show little resemblence with the exact results. Enhancement of hopping anisotropy by Hund's rule correlations are found in all approximations.Comment: 9 pages, 9 figure

Competition between Kondo screening and quantum Hall edge reconstruction

We report on a Kondo correlated quantum dot connected to two-dimensional leads where we demonstrate the renormalization of the g-factor in the pure Zeeman case i.e, for magnetic fields parallel to the plane of the quantum dot. For the same system we study the influence of orbital effects by investigating the quantum Hall regime i.e. a perpendicular magnetic field is applied. In this case an unusual behaviour of the suppression of the Kondo effect and of the split zero-bias anomaly is observed. The splitting decreases with magnetic field and shows discontinuous changes which are attributed to the intricate interplay between Kondo screening and the quantum Hall edge structure originating from electrostatic screening. This edge structure made up of compressible and incompressible stripes strongly affects the Kondo temperature of the quantum dot and thereby influences the renormalized g-factor

Lifshitz transitions and quasiparticle de-renormalization in YbRh2_2Si2_2

We study the effect of magnetic fields up to 15 T on the heavy fermion state of YbRh$_2$Si$_2$ via Hall effect and magnetoresistance measurements down to 50 mK. Our data show anomalies at three different characteristic fields. We compare our data to renormalized band structure calculations through which we identify Lifshitz transitions associated with the heavy fermion bands. The Hall measurements indicate that the de-renormalization of the quasiparticles, {\it i.e} the destruction of the local Kondo singlets, occurs smoothly while the Lifshitz transitions occur within rather confined regions of the magnetic field.Comment: 7 pages, 5 figure

Similar temperature scale for valence changes in Kondo lattices with different Kondo temperatures

The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy T_K of the Kondo interaction. Here, we study the evolution of the 4f occupancy with temperature in a series of Yb Kondo lattices using resonant X-ray emission spectroscopy. In agreement with simple theoretical models, we observe a scaling between the valence at low temperature and T_K obtained from thermodynamic measurements. In contrast, the temperature scale T_v at which the valence increases with temperature is almost the same in all investigated materials while the Kondo temperatures differ by almost four orders of magnitude. This observation is in remarkable contradiction to both naive expectation and precise theoretical predictions of the Kondo model, asking for further theoretical work in order to explain our findings. Our data exclude the presence of a quantum critical valence transition in YbRh2Si2