<p>The present thesis concerns method development and applications in the field of first principles electronic structure calculations.</p><p>Augmented planewaves combine the simple planewaves with exact solutions of the Schrödinger equation for a spherical potential. This combination yields a very good set of basis functions for describing the electronic structure everywhere in a crystal potential. In the present work, developments of the original augmented planewave (APW) method are presented. It is shown that the exact APW eigenvalues can be found using information from the eigenvalues of the APW secular matrix. This provides a more efficient scheme to solve the APW eigenvalue problem, than the traditional evaluation of the secular determinant. Further, a new way of linearizing the APW method is presented and compared to the traditional linearized APW method (LAPW). Using a combination of the original APW basis functions and the so called local orbitals (lo), the APW+lo linearization is found to reproduce the results of the LAPW method, but already at a smaller basis set size. Another advantage of the new linearization is a faster convergence of forces, with respect to the basis set size, as compared to the LAPW method.</p><p>The applications include studies of the non-collinear magnetic configuration in the fcc-based high-temperature phase of iron, γ-Fe. The system is found to be extremely sensitive to volume changes, as well as to a tetragonal distortion of the cubic unit cell. A continuum of degenerate spin spiral configurations, including the global energy minimum, are found for the undistorted crystal. The in-plane anisotropy of the ideal interface between a ferromagnetic layer of bcc Fe and the semiconducting ZnSe crystal is also investigated. In contrast to the four-fold symmetric arrangement of the atoms at the interface, the in-plane magnetic anisotropy displays a large uniaxiality. The calculated easy axes are in agreement with experiments for both Se and Zn terminated interfaces. In addition, calculations of the hyperfine parameters were performed for Li intercalated battery materials.</p>

The present thesis concerns method development and applications in the field of first principles electronic structure calculations. Augmented planewaves combine the simple planewaves with exact solutions of the Schrödinger equation for a spherical potential. This combination yields a very good set of basis functions for describing the electronic structure everywhere in a crystal potential. In the present work, developments of the original augmented planewave (APW) method are presented. It is shown that the exact APW eigenvalues can be found using information from the eigenvalues of the APW secular matrix. This provides a more efficient scheme to solve the APW eigenvalue problem, than the traditional evaluation of the secular determinant. Further, a new way of linearizing the APW method is presented and compared to the traditional linearized APW method (LAPW). Using a combination of the original APW basis functions and the so called local orbitals (lo), the APW+lo linearization is found to reproduce the results of the LAPW method, but already at a smaller basis set size. Another advantage of the new linearization is a faster convergence of forces, with respect to the basis set size, as compared to the LAPW method. The applications include studies of the non-collinear magnetic configuration in the fcc-based high-temperature phase of iron, γ-Fe. The system is found to be extremely sensitive to volume changes, as well as to a tetragonal distortion of the cubic unit cell. A continuum of degenerate spin spiral configurations, including the global energy minimum, are found for the undistorted crystal. The in-plane anisotropy of the ideal interface between a ferromagnetic layer of bcc Fe and the semiconducting ZnSe crystal is also investigated. In contrast to the four-fold symmetric arrangement of the atoms at the interface, the in-plane magnetic anisotropy displays a large uniaxiality. The calculated easy axes are in agreement with experiments for both Se and Zn terminated interfaces. In addition, calculations of the hyperfine parameters were performed for Li intercalated battery materials.

L’objectif de cette thèse est l'étude par spectroscopie laser colinéaire à haute résolution de la structure nucléaire des isotopes d’étain riches en neutrons, vers de la fermeture de couche N=82 et au-delà. Les structures hyperfines et les déplacements isotopiques le long de ¹⁰⁸⁻¹³⁴Sn ont été mesurés en utilisant l’expérience COLLAPS à ISOLDE au CERN. Deux expériences indépendantes, utilisant des propriétés de transitions complémentaires l’une à 452 et l’autre à 286 nanomètres, ont étudiées les états 5p6s ¹P₁ et 5p6s ³P₁ dans l'atome neutre. L'état singlet fournit une sensibilité élevée au moment quadrupolaire tandis que le triplet facilite une grande séparation magnétique. A partir d'une analyse auto-cohérente des deux ensembles de données, les spins nucléaires, les moments électromagnétiques et les rayons de charge ont été extraits. Les propriétés des isomères à vie longue des noyaux ¹¹³Sn, ¹²³Sn, ¹²⁸Sn ainsi que l'état fondamental de ¹³³Sn et ¹³⁴Sn ont été évalués pour la première fois. Les moments quadrupolaires des états 11/2⁻, déterminés avec une plus grande précision que les études précédentes, suivent une tendance presque linéaire. Un coude à N=82 dans la courbe des rayons a été observé pour la première fois. Des calculs de champ moyen fournissent une description précise des rayons et relient en outre la tendance globale aux corrélations provenant des fluctuations des moments quadrupolaires. / The aim of this thesis is the study of nuclear structure properties of the neutron-rich Sn isotopes towards the N=82 shell closure and beyond by high-resolution collinear laser spectroscopy. The hyperfine structures and isotope shifts along ¹⁰⁸⁻¹³⁴Sn were measured using the COLLAPS instrumentation at ISOLDE, CERN. Two independent experiments using transitions with complementary properties, respectively at 452 and 286 nanometres studied the 5p6s ¹P₁ and the 5p6s ³P₁ states in the neutral atom. The singlet state provided high sensitivity to quadrupole moments while the triplet facilitated a large magnetic splitting. From a self-consistent analysis of the two data sets, nuclear spins, electromagnetic moments and charge radii have been extracted. The properties of the long-lived isomers in ¹¹³Sn, ¹²³Sn, ¹²⁸Sn and the ground state of ¹³³Sn and ¹³⁴Sn have been assessed for the first time. The quadrupole moments of the 11/2⁻ states, determined with much higher precision than in previous studies, have been found to follow a nearly linear trend. A "kink" in the radii trend at N=82 was observed for the first time. Beyond mean-field calculations provide an accurate description of the radii and further relate the overall trend to correlations stemming from the fluctuations of the quadrupole moments.