La skutterudite PrOs4Sb12: supraconductivité et corrélations

The filled skutterudite PrOs4Sb12 is the first Pr-based heavy fermion superconductor. This thesis addresses several important open questions including the determination of the quasi-particle mass renormalisation, the nature and mechanism of superconductivity, and the intrinsic or extrinsic nature of the double superconducting transition seen in the specific heat. A fit of the specific heat with magnetic interactions between the ions Pr is proposed. We extract from it an electronic term of between 300-750mJ/K2.mol(Pr). Analysis of the specific heat jump provides evidence that heavy carriers are involved in Cooper pairing and that superconductivity is strongly coupled. Extensive characterisations by specific heat, resistivity, susceptibility measurements show that a double transition appears in the best samples. Nevertheless we bring the first serious doubts on the intrinsic nature of the double transition, because we have found samples with a single sharp transition at Tc2 and because the ratio of the two specific heat jumps shows strong dispersion among the samples. Furthermore we have measured the superconducting phase diagrams with an A.C. specific heat technique under magnetic field and under pressure up to 4.2 GPa, and we show that the two transitions, Tc1 and Tc2, exhibit similar behaviours with magnetic field and pressure.We find a strong change in the pressure dependence of Tc's above 2 GPa which might be related to a change in the nature of the superconductivity under pressure (at least partially mediated by fluctuations and only by phonons at respectively low and high pressure) which may be linked to the increase of the crystal field gap of the Pr ions. Analysis of the upper critical field shows the presence of at least two superconducting bands and concludes to a singlet nature of the pairing. A strong distortion of the flux-line lattice, which is constant with temperature and field, is obtained by small angle neutron scattering measurement. Further measurement or calculation are needed to distinguish between the explanation based on the presence of nodes in the superconducting gap and the analysis based on the topology of the Fermi surface in a Th symmetry.La skutterudite PrOs4Sb12 est le premier composé à fermion lourd supraconducteur à base de Praséodyme. Cette thèse s'attache à répondre à plusieurs questions le concernant comme la détermination de l'intensité de la renormalisation de la masse des quasi-particules, la nature et le mécanisme à l'origine de la supraconductivité et la nature intrinsèque ou extrinsèque de la double transition supraconductrice vue en chaleur spécifique. Nous proposons une interpolation de la chaleur spécifique en phase normale en tenant compte des interactions magnétiques entre ions Pr. Nous extrayons alors un terme électronique de chaleur spécifique compris entre 300 et 750mJ/K2.mol(Pr). L'analyse du saut en chaleur spécifique à la transition supraconductrice confirme que les quasi-particules lourdes sont impliquées dans la supraconductivité et que la supraconductivité est en régime de couplage fort. Des caractérisations systématiques par chaleur spécifique, résistivité et susceptibilité indiquent que la double transition apparaît dans les meilleurs échantillons. Néanmoins nous apportons les premiers doutes sérieux sur sa nature intrinsèque, parce que nous avons trouvé plusieurs échantillons avec une unique transition étroite et parce qu'une forte dispersion dans la valeur du rapport des deux sauts en chaleur spécifique a été mise en évidence. De plus, en établissant les diagrammes de phase supraconducteurs sous champ magnétique et sous pression jusqu'à 4.2 GPa par chaleur spécifique alternative, nous montrons que les deux transitions supraconductrices Tc1 et Tc2 présentent des comportements similaires. Nous avançons l'hypothèse que le fort changement dans l'évolution des Tc sous pression au dessus de 2 GPa est dû à un changement de nature de la supraconductivité (impliquant des fluctuations puis uniquement phononique à respectivement basse et haute pression) en lien avec l'augmentation du gap de champ cristallin des ions Pr sous pression. L'analyse du second champ critique Hc2(T) montrent la présence d'au moins deux bandes supraconductrices et conclue à la nature singulet du spin des paires de Cooper. Une forte distorsion du réseau de vortex, constante avec le champ et la température, est obtenue par diffraction de neutrons. Des mesures supplémentaires ou un nouveau calcul seraient nécessaires pour trancher entre une explication basée sur la présence de zéros dans le gap supraconducteur et une analyse basée sur la topologie de la surface de Fermi en symétrie Th

Raman Scattering as a Selective Probe of Chiral Electronic Excitations in Bilayer Graphene

We report a symmetry resolved electronic Raman scattering (ERS) study of a bilayer graphene device under gate voltage. We show that the ERS continuum is dominated by interband chiral excitations of $A_{2}$ symmetry and displays a characteristic Pauli-blocking behavior similar to the monolayer case. Crucially, we show that non-chiral excitations make a vanishing contribution to the Raman cross-section due to destructive interference effects in the Raman amplitude matrix elements. This is in a marked contrast to optical absorption measurements and opens interesting venues for the use of Raman scattering as a selective probe of chiral degrees of freedom in topological matter and other 2D crystals

Oscillating Nernst-Ettingshausen effect in Bismuth across the quantum limit

In elemental Bismuth, 10$^5$ atoms share a single itinerant electron. Therefore, a moderate magnetic field can confine electrons to the lowest Landau level. We report on the first study of metallic thermoelectricity in this regime. The main thermoelectric response is off-diagonal with an oscillating component several times larger than the non-oscillating background. When the first Landau level attains the Fermi Energy, both the Nernst and the Ettingshausen coefficients sharply peak, and the latter attains a temperature-independent maximum. A qualitative agreement with a theory invoking current-carrying edge excitations is observed.Comment: Final published versio

Higgs-mode radiance and charge-density-wave order in 2H-NbSe2_2

Despite being usually considered two competing phenomena, charge-density-wave and superconductivity coexist in few systems, the most emblematic one being the transition metal dichalcogenide 2H-NbSe$_2$. This unusual condition is responsible for specific Raman signatures across the two phase transitions in this compound. While the appearance of a soft phonon mode is a well-established fingerprint of the charge-density-wave order, the nature of the sharp sub-gap mode emerging below the superconducting temperature is still under debate. In this work we use the external pressure as a knob to unveil the delicate interplay between the two orders, and consequently the nature of the superconducting mode. Thanks to an advanced extreme-conditions Raman technique we are able to follow the pressure evolution and the simultaneous collapse of the two intertwined charge density wave and superconducting modes. The comparison with microscopic calculations in a model system supports the Higgs-type nature of the superconducting mode and suggests that charge-density-wave and superconductivity in 2H-NbSe$_2$ involve mutual electronic degrees of freedom. These findings fill knowledge gap on the electronic mechanisms at play in transition metal dichalcogenides, a crucial step to fully exploit their properties in few-layers systems optimized for devices applications

Anharmonic suppression of Charge density wave in 2H-NbS2_2

The temperature dependence of the phonon spectrum in the superconducting transition metal dichalcogenide 2H-NbS$_2$ is measured by diffuse and inelastic x-ray scattering. A deep, wide and strongly temperature dependent softening, of the two lowest energy longitudinal phonons bands, appears along the $\mathrm{\Gamma M}$ symmetry line in reciprocal space. In sharp contrast to the iso-electronic compounds 2H-NbSe$_2$, the soft phonons energies are finite, even at very low temperature, and no charge density wave instability occurs, in disagreement with harmonic ab-initio calculations. We show that 2H-NbS$_2$ is at the verge of the charge density wave transition and its occurrence is only suppressed by the large anharmonic effects. Moreover, the anharmonicity and the electron phonon coupling both show a strong in-plane anisotropy.Comment: 6 pages, 5 figures, accepted for publication in Physical Review

Nernst effect in semi-metals: the meritorious heaviness of electrons

We present a study of electric, thermal and thermoelectric transport in elemental Bismuth, which presents a Nernst coefficient much larger than what was found in correlated metals. We argue that this is due to the combination of an exceptionally low carrier density with a very long electronic mean-free-path. The low thermomagnetic figure of merit is traced to the lightness of electrons. Heavy-electron semi-metals, which keep a metallic behavior in presence of a magnetic field, emerge as promising candidates for thermomagnetic cooling at low temperatures.Comment: 4 pages, including 4 figure

Collapse of critical nematic fluctuations in FeSe under pressure

We report the evolution of the electronic nematic susceptibility in FeSe via Raman scattering as a function of hydrostatic pressure up to 5.8 GPa where the superconducting transition temperature $T_{c}$ reaches its maximum. The critical nematic fluctuations observed at low pressure vanish above 1.6 GPa, indicating they play a marginal role in the four-fold enhancement of $T_{c}$ at higher pressures. The collapse of nematic fluctuations appears to be linked to a suppression of low energy electronic excitations which manifests itself by optical phonon anomalies at around 2 GPa, in agreement with lattice dynamical and electronic structure calculations using local density approximation combined with dynamical mean field theory. Our results reveal two different regimes of nematicity in the phase diagram of FeSe under pressure: a d-wave Pomeranchuk instability of the Fermi surface at low pressure and a magnetic driven orthorhombic distortion at higher pressure.Comment: 7 pages, 4 figures. Supplementary Material available upon reques

Lattice dynamics in the intermetallic LaFeSi and the derived superconducting compounds LaFeSiH and LaFeSiO

The intermetallic LaFeSi and the derived superconducting compounds LaFeSiH and LaFeSiO have been investigated by polarized Raman spectroscopy. The frequency and symmetry of the Raman phonons modes are well-reproduced by ab-initio calculations. The ionic character of the spacer in this series of compounds and its coupling with the FeSi layers as compared to As-based compounds are discussed. Already at room temperature, Fano-shape modes are reported in the A1g channel while an intriguing doubling of the Fe-based B1g phonon is measured in LaFeSiH. Origins of these observations are discussed based on electron diffraction data and the different scenarios for the origin of such splitting are explored. Furthermore, there is no signature of a structural transition nor long range magnetic ordering in LaFeSiH down to 9 K.Comment: 8 pages, 6 figures