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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
51

Study on the Electronic Band Structure of the Spinel Superconductor LiTi2O4 / Studie om den Elektroniska Bandstrukturen hos Spinel Supraledaren LiTi2O4

Di Berardino, Gaia January 2022 (has links)
This master’s thesis focuses on investigating the electronic properties of the superconducting spinel compound LiTi2O4 by means of computational and experimental effort. The title compound has been extensively studied in the past years, being the only known superconducting spinel oxide with relatively high Tc = 11.5 K. Even so, the origin of its superconducting mechanism is under debate, and its anomalous superconductivity is still inquired. Thanks to the recently developed ability to produce high-quality epitaxial LiTi2O4 thin films, a renewed research interest in this compound has matured. With this work, we partake in this challenge and present combined experimental and computational results on the electronic band structure of the material. Density functional theory (DFT) has been employed for the first principle electronic structure calculations performed with the Quantum ESPRESSO software. Furthermore, thin-film samples were in-situ realized with the pulsed laser deposition (PLD) method and investigated through the angle-resolved photoemission spectroscopy (ARPES) technique conducted at the ULTRA end-station of the SLS synchrotron facility at PSI in Switzerland. Here, we report the computed electronic band structure of LiTi2O4, with a detailed investigation of its density of states and Fermi surface. Further, we compare these calculations with the obtained experimental ARPES data. Emerging from this study are results supporting the non-conventional superconducting nature of LiTi2O4, which presents coexisting correlation effects, such as electron-phonon coupling and enhanced electron-electron interactions. / Denna masteruppsats fokuserar på att undersöka de elektroniska egenskaperna hos det supraledande spinellmaterialet LiTi2O4 med hjälp av datorsimuleringar samt experimentella mätningar. LiTi2O4 har studerats omfattande under de senaste åren, eftersom den är den enda kända supraledande spinelloxiden med relativt hög Tc = 11.5 K. Trots det är ursprunget till dess supraledande mekanism debatterad, och meaknismen för dess okonventionella supraledning är fortfarande inte helt förstådd. Tack vare den nyligen utvecklade förmågan att producera tunna högkvalitativa epitaxiella LiTi2O4 filmer, har ett förnyat forskningsintresse för denna förening mognat. Med detta arbete deltar vi i denna utmaning och presenterar kombinerade experimentella och beräkningsresultat om materialets elektroniska bandstruktur. Densitetsfunktionsteori (DFT) har använts för principiella elektroniska strukturberäkningar utförda med Quantum ESPRESSO-mjukvaran. Vidare realiserades tunnfilmsprover in-situ med pulsed laser deposition (PLD) medoden och undersöktes experimentellt via vinkelupplöst fotoemissionsspektroskopi (ARPES) som utfördes vid ULTRA-ändstationen på SLS synkrotronanläggningen vid PSI i Schweiz. Här rapporterar vi den beräknade elektroniska bandstrukturen för LiTi2O4, med en detaljerad undersökning av dess tillståndstäthet och Fermi-yta. Vidare jämför vi dessa teoretiska beräkningar med de erhållna experimentella ARPES data. Resultat från denna studie stöder den icke-konventionella supraledande naturen hos LiTi2O4, som också uppvisare samexisterande korrelationseffekter, såsom elektron-fononkoppling samt starka elektron-elektron-interaktioner.
52

Unexpected temperature and polarization behavior of the high-TC superconductor Bi(Pb)-2212

Ghafari, Aliakbar 03 June 2013 (has links)
In dieser Doktorarbeit wird der Hochtemperatur-Supraleiter Bi-2212 auf seine elektronische Struktur hin untersucht. Für diesen Zweck wurden Röntgen- Absorptionsspektroskopie (XAS) und winkelaufgelöste Photoemissionsspektroskopie (ARPES) verwendet. Zusätzlich wurden mittels Dichtefunktionaltheorie theoretische Trends in der elektronischen Struktur aufgezeigt. Zu Beginn wurde die Temperaturabhängigkeit der Löcher-Konzentration (nH) von nahezu optimal dotierten und geringfügig unterdotierten Einkristallen mittels XAS untersucht. Die Messungen der Temperaturabhängigkeit von nH mit XAS zeigen ein komplett anderes Verhalten als das, welches aus dem Hall-Effekt hergeleitet wurde. Hinzu kommt, dass es unmöglich ist, die Formel von Gor''kov und Teitel''baum, d.h. mit einem konstanten und einem Aktivierungsterm, an die Daten anzupassen. Als Lösungsansatz kommen Magnonen in Frage. Zusätzlich wurde die Polarisationsabhängigkeit der Löcher- Konzentration mittels XAS gemessen, die zeigt, dass in den Kupferoxidschichten die Löcher offenbar offenbar inhomogen verteilt sind. Solch ein Verhalten wird für die isotrope Struktur der Bi-2212-Kristalle nicht erwartet und kann nur schwer erklärt werden. Möglicherweise sind die, die Symmetrie brechenden magnetischen Eigenschaften wie magnetische Streifen die Antwort. Um zusätzliche experimentelle Informationen zu erhalten, wurde darüber hinaus noch die Temperatur- und Polarisationsabhängigkeit der Bi-2212-Einkristalle mittels ARPES studiert. Insbesondere die ''Peak-Dip-Hump''-Emissionsstruktur an der Fermi-Energie wurde gemesssen, die sich am M-Punkt der Brillouin-Zone befindet. Die Ergebnisse zeigen, dass der scharfe Peak nahe der Fermi-Kante eine deutliche Polarisations- und Temperaturabhängigkeit aufweist, welche bei der Pseudolücken-Temperatur T* und nicht bei der Sprungtemperatur TC verschwindet. Die Polarisationsabhängigkeit an den vier M-Punkten der Brillouin-Zone hat gezeigt, dass eine Symmetrieachse im 45°-Winkel zur Cu-O-Cu-Richtung existiert. Dies könnte ebenfalls mit magnetischer Streifenbildung erklärt werden. Des Weiteren wurde das beobachtete Versagen der Dipol-Näherung zur Beschreibung der Spektren bei einer Polarisation senkrecht zur Spiegelebene erörtert. Andererseits ist die Berechnung von Materieleigenschaften mittels der Dichtefunktionaltheorie ein sehr aktiver Bereich der Festkörperphysik geworden. Nachdem meine DFT-Rechnungen auf der Basis des MBJ-Potentials sehr gute Übereinstimmung mit den experimentellen Ergebnissen des ternären Halbleiters ZrSexS2-x und die LiZrSexS2-x –Verbindung erzielt haben, habe ich diese auch zur Unterstützung der experimentellen Supraleiterdaten angewendet. Die elektronischen Eigenschaften von CaCuO2 und des Bi-2212-Kuprats wurden mittels DFT auf der Basis von GGA und GGA+U berechnet, wobei der Hubbard-U-Term mit einer „abinitio“-Methode berechnet wurde. Die Ergebnisse ergaben, dass nur Rechnungen auf der Basis von MBJ+U einen antiferromagnetischen Grundzustand für die CaCuO2- Verbindung lieferten, während alle Funktionale versagten, den antiferromagnetischen Grundzustand für das Bi-2212-Kuprat zu finden. / In this PhD work the electronic structure of high-TC Bi-2212 cuprates is investigated. For this purpose x-ray absorption spectroscopy (XAS) and angle resolved photoemission spectroscopy (ARPES) are used. Additionally, density functional theory is applied for making theoretical trends of the electronic structure evident. At first, the temperature dependence of the hole density (nH) by XAS on nearly optimum and slightly underdoped single crystals is studied. The measurements of the temperature dependence of nH by XAS show completely different behavior as that derived from Hall effect. Moreover, fitting our data by the Gor’kov and Teitel’baum formula, i.e. assuming a constant term and an activation term, was impossible. For solving the problem a contribution of magnons is suggested. Additionally, the polarization dependence of the hole density has been measured by XAS showing that an inhomogeneity of holes in the copper oxide planes may exist. Such a behavior is not expected for the isotropic structure of the Bi(Pb)-2212 crystals and was only hardly to be explained. Possibly, magnetic symmetry breaking properties like e.g. magnetic stripes might give an answer. In order to derive additional experimental information, the temperature and polarization dependence of the electronic structure of the CuO2 planes of Bi(Pb)-2212 single crystals has been studied by ARPES. In particular, the so-called peak-dip-hump emission structure close to the Fermi energy has been measured, which is located at the M point of the Brillouin zone. The results show that the sharp emission structure close to the Fermi edge reveals a distinct polarization dependence and it vanishes at the pseudogap temperature T* and not at the critical temperature TC. The polarization dependence at the four M points of the Brillouin zone has revealed that there exists a symmetry line along to 45?? from the Cu-O-Cu direction. This could also be due to stripe formation. Additionally, the observed failure of the dipole approximation to describe the spectra at normal polarization with respect to the mirror plane is discussed. On the other hand, the calculation of material properties by density functional theory has become a very active area of research in condensed matter physics. Therefore, after my calculations based on DFT by the MBJ potential have revealed good agreement with experimental data for the ternary semiconductors ZrSexS2-x and the LiZrSexS2-x compound I applied it for a support of the experimental superconductor data. The electronic properties of CaCuO2 and the Bi-2212 cuprate have been calculated by DFT based on GGA and GGA+U where the Hubbard U term has been calculated by an ab initio method. The results reveal that only calculations based on MBJ+U lead to an anti-ferromagnetic ground state for the CaCuO2 compound while all functionals fail to find an antiferromagnetic ground state for Bi-2212.
53

Propriétés électroniques et de transport du semi-métal corrélé quasi-2D BaNiS2 / Electronic and transport properties of the quasi-2D correlated semimetal BaNiS2

Santos-Cottin, David 08 April 2015 (has links)
Ce travail de thèse a pour but de clarifier le mécanisme de la transition métal-isolant (MIT) pilotée par le dopage électronique x du système quasi-2D BaCo1-xNixS2.Une optimisation de la croissance de monocristaux pour des taux de substitution allant de x = 0 à 1 a été nécessaire. Cela a permis de synthétiser de manière reproductible des monocristaux non lacunaires en soufre, de taille millimétrique et de haute qualité. L'analyse structurale de ces cristaux a permis d'établir une relation précise entre les distances métal-soufres et le taux de substitution x.Le travail de thèse a ensuite été focalisé sur l'étude des propriétés électroniques et de transport de BaNiS2 la phase métallique précurseur de la MIT. Les études de la structure électronique par photoémission résolue en angle (ARPES) et par des mesures d'oscillations quantiques ont révélées une surface de Fermi composée d'une poche d'électrons 2D centrée en Γ(Z) et d'une poche de trous positionnée à mi-distance suivant ΓM(ZA) quasi-2D avec une dispersion conique à kz =0. Une levée de dégénérescence des bandes à Γ et à X révèle la présence inattendue et importante d'un couplage spin-orbite et d'un couplage Rashba. Les mesures de magnétotransport ont pu être expliquées par un modèle qui implique que BaNiS2 est un semi-métal compensé avec trois voies de conduction. Des trous p1 et électrons e1 largement majoritaires et présentant des mobilités modérées ainsi que des trous p2 minoritaires de très haute mobilité.La cohérence de l'ensemble des mesures donne une image précise de la surface de Fermi de BaNiS2 et de ses propriétés électroniques plus bidimensionnelle que celle prévu par le calculs de bandes conventionnelle. / This work aims to clarify the mechanism of the metal-insulator transition (MIT) driven by doping x in the quasi-2D BaCo1-xNixS2 system. First of all, synthesize of high quality single crystals with substitution level x varying in the full 0 - 1 range was fundamental. It appears that the mechanism of the metal-insulator transition is associated to a continuous modification of metal-sulfurs distances. Then, we focus on an investigated the electronic properties of BaNiS2, precursor metallic phase of the MIT. Studies of the electronic structure of BaNiS2 by angle-resolved photoemission spectroscopy (ARPES) and by quantum oscillation measurements reveal the existence of two pockets at the Fermi surface: an electron-like 2D pocket centered in Γ(Z) and a hole-like pocket quasi-2D at mi-distance along ΓM(ZA) with a conic-like dispersion in kz = 0 . Furthermore, data also show a very large spin-orbit splitting at Γ and Z which is unexpected in a 3d metal compound. From previous studies, we developed a model to explain magnetotransport properties of BaNiS2. This model involves that BaNiS2 is a three carriers compensated metal: a majority holes p1 and electrons e1 carriers with moderate mobilities and a minor holes p2 carriers with a high mobility. The two different holes carries observed in magneto-transport could be explain by an important variation of the hole-like pocket dispersion along kz. Measures realized during this thesis are consistent and allowed to know precisely the form of the Fermi surface of BaNiS2 and its electronic properties which are more bi-dimensional than predict by conventional calculation.
54

Polarization doping of graphene on silicon carbide

Mammadov, Samir, Ristein, Jürgen, Koch, Roland J., Ostler, Markus, Raidel, Christian, Wanke, Martina, Vasiliauskas, Remigijus, Yakimova, Rositza, Seyller, Thomas 07 May 2018 (has links)
The doping of quasi-freestanding graphene (QFG) on H-terminated, Si-face 6H-, 4H-, and 3C-SiC is studied by angle-resolved photoelectron spectroscopy (ARPES) close to the Dirac point. Using semi-insulating as well as n-type doped substrates we shed light on the contributions to the charge carrier density in QFG caused by i) the spontaneous polarization of the substrate, and ii) the band alignment between the substrate and the graphene layer. In this way we provide quantitative support for the previously suggested model of polarization doping of graphene on SiC [Phys. Rev. Lett. 108, 246104 (2012)].
55

Bulk electronic structure of single-crystal perovskite oxides studied by soft X-ray angle-resolved photoemission.

Falke, Johannes 14 May 2024 (has links)
The transition-metal oxides (TMOs) are a material class host to a number of intriguing and potentially technologically useful phenomena as a result of many-body correlation effects, from superconductivity, magnetic and orbital ordering, to ferroelectricity and metal-insulator transitions. Here, materials with similar structures and seemingly equivalent electronic configuration often exhibit wildly different properties as a result of strong competition between different ground states from the many degrees of freedom, whose balance can be further tuned through the use of pressure, doping, magnetic fields or temperature. To investigate these materials, we make use of photoelectron spectroscopy (PES), probing elementary excitations possible in the material and thus providing linked information both about the ground state and possible excited states, closely related to the physical properties of a material such as its response to external fields. Angle-resolved PES (ARPES) provides additional momentum information and as a result, it is uniquely suited to investigate the character of the electronic structure of solids as it resolves the dispersion, meaningful in the independent-electron view where crystal momentum is a well-defined quantum number, but which can retain validity even in strongly correlated systems through the concept of quasiparticles. While ARPES is a well-established technique, it is rarely used in the soft X-ray regime (SX-ARPES) due to significant experimental challenges posed. However, the higher energies in SX-ARPES allow it to be significantly more bulk-sensitive, an extremely important fact since the properties of the bulk material and its surface are often extremely, or worse, subtly different. Critically, this permits measurements on single crystals of TMOs, whose surfaces may show roughness or reconstruction, for example as a result of a polar surface compensation, but whose bulk properties are well-defined in contrast to thin films which are additionally subject to substrate effects. We demonstrate on three rather different perovskite oxides, a three-dimensional class of TMOs, that is worthwhile to overcome these issues since it provides access to the true momentum-resolved bulk electronic properties of materials and allows filling noticeable gaps in literature of k-resolved electronic structure measurements for this class of compounds stemming from the impossibility of such measurements at lower energy. A commonality between the materials studied in this thesis is the absence of a strong electronic symmetry-breaking order, such as local-moment antiferromagnetism or charge ordering, that could suppress the existence of sufficiently long-lived quasiparticles to observe dispersion (or equivalently prevent a mobile photo-hole). We first establish that SX-ARPES is indeed capable and suited to measure the bulk-representative electronic structure by measurements on the perfect cubic d1 perovskite ReO3. We present the first k-resolved electronic structure for this material which is rather well explained by band structure, especially close to the Fermi level. In particular, we show and quantify the impact of the significant spin-orbit coupling on the Fermi surface and bands. However, the oxygen bands are less well reproduced by calculations and are correctable by use of hybrid functionals, taken as a sign of spurious self-interaction effects - likely due to the large extent and density differences between delocalised Re 5d and more localised O 2p. We also show that there are signs of some hitherto unknown distortion in ReO3. We then turn to LaNiO3, a metallic oxide in a family of formally d7 rare-earth nickelates which otherwise all undergo metal-insulator and antiferromagnetic (AFM) transitions as well as oxygen bond disproportionation, with a strong competition between these ground states and possible exotic resulting states in the phase diagram. We are able to resolve the dispersion of the eg quasiparticle spectrum along high symmetry cuts of this material as well as its Fermi surface, the latter of which is accurately reproduced by band theory calculations. We investigate the influence of the rhombohedral distortion present in the material through unfolding methods to better compare their influence to measurement, and show how significantly it affects the dispersion, confirming again the importance of single crystals. Its effects are shown to be similar to correlation-induced mass enhancement and their effects are untangled with the help of first DFT+U and later rhombohedral multi-band dynamical mean-field theory (DMFT) calculations. Local correlation effects prove to be the dominant influence on the spectrum, although certain k-dependent mismatches remain, pointing to a possible simultaneous importance of non-local mechanisms. Finally, on the d6 system LaCoO3 that is close to a spin-state transition, we show that this method can also be applied to insulating oxides. Absent a Fermi surface, we naturally concentrate more on the full valence band, where we show that the observed dispersion is well-described by mean-field band methods in the low-spin (LS) regime of LaCoO3 provided that static energy corrections of DFT+U are accounted for (which show a good match to local LS many-body configuration interaction calculations), thus providing k-resolved evidence that one may effectively consider LS LaCoO3 a band insulator, despite possibly strong correlations. We further unveil clear evidence of crystal periodicity doubling by observation of a backfolded oxygen band, and show evidence of a significant asymmetry in the k-resolved lineshape in the valence band and lastly we take a look at the spin state of Co at the surface, which, contrary to prior results, appears to be the same as in the bulk, but which we show to be complicated by significant orbital-shape matrix element effects.
56

Thin Mn silicide and germanide layers studied by photoemission and STM

Hirvonen Grytzelius, Joakim January 2012 (has links)
The research presented in this thesis concerns experimental studies of thin manganese silicide and germanide layers, grown by solid phase epitaxy on the Si(111)7×7 and the Ge(111)c(2×8) surfaces, respectively. The atomic and electronic structures, as well as growth modes of the epitaxial Mn-Si and Mn-Ge layers, were investigated by low-energy electron diffraction (LEED), angle-resolved photoelectron spectroscopy (ARPES), core-level spectroscopy (CLS), and scanning tunneling microscopy and spectroscopy (STM and STS). The magnetic properties of the Mn-Ge films were investigated by X-ray magnetic circular dichroism (XMCD). The Mn-Si layers, annealed at 400 °C, showed a √3×√3 LEED pattern, consistent with the formation of the stoichiometric monosilicide MnSi. Up to 4 monolayers (ML) of Mn coverage, island formation was observed. For higher Mn coverages, uniform film growth was found. Our results concerning morphology and the atomic and electronic structure of the Mn/Si(111)-√3×√3 surface, are in good agreement with a recent theoretical model for a layered MnSi structure and the √3×√3 surface structure. Similar to the Mn-Si case, the grown Mn-Ge films, annealed at 330 °C and 450 °C, showed a √3×√3 LEED pattern. This indicated the formation of the ordered Mn5Ge3 germanide. A strong tendency to island formation was observed for the Mn5Ge3 films, and a Mn coverage of about 32 ML was needed to obtain a continuous film. Our STM and CLS results are in good agreement with the established model for the bulk Mn5Ge3 germanide, with a surface termination of Mn atoms arranged in a honeycomb pattern. Mn-Ge films grown at a lower annealing temperature, 260 °C, showed a continuous film at lower coverages, with a film structure that is different compared to the structure of the Mn5Ge3 film. XMCD studies showed that the low-temperature films are ferromagnetic for 16 ML Mn coverage and above, with a Curie temperature of ~250 K.
57

Gestufte Cu-Oberflächen und Ag-Nano-Streifen: atomare und elektronische Struktur

Bachmann, Andreas R. 15 November 2002 (has links)
I. Atomare Struktur Mittels Rastertunnelmikroskopie und Beugung langsamer Elektronen wird die atomare Struktur von vizinalen Cu(111)-Oberflächen untersucht. Der mittlere Stufenabstand auf den untersuchten Oberflächen deckt einen Bereich von ca. 1.0-2.5nm ab. Auf allen diesen Oberflächen wird ein regelmäßiges Stufenarray gefunden.Es wird gezeigt, dass das System Ag/Cu(223) ein gutes Beispiel für den Effekt der Selbstorganisation auf Kristalloberflächen darstellt. Durch die Ag-Adsorption im Bereich von 0-1ML wird eine periodische Facettierung der Cu(223)-Oberfläche induziert. Die Gleichgewichtsstruktur setzt sich aus Ag-bedeckten Facetten zusammen, die mit reinen Cu-Streifen alternieren. Die Breite der Cu- und der Ag-Streifen kann in einem Bereich von 3-30nm über die Ag-Bedeckung kontinuierlich eingestellt werden. II. Elektronische Struktur Mittels winkelaufgelöster Photoelektronen-Spektroskopie mit Synchrotron-Strahlung wird der Einfluss von Stufen auf den Oberflächenzustand von vizinalen Cu(111)-Oberflächen untersucht. Veränderungen bzgl. der Bindungsenergie werden im Rahmen eines eindimensionalen Kronig-Penny-Modells interpretiert. Als Ursache für das Kippen der Ausbreitungsebene bei einer kritischen Terrassenbreite (~1.7nm) wird die Überlagerung des Oberflächenzustands mit Volumenzuständen und dem damit verbundenen Übergang zur Oberflächenresonanz diskutiert. Bei dem System Ag/Cu(223) wird der Oberflächenzustand innerhalb der Cu-Streifen zum einen durch die Ag-Streifen lateral begrenzt, zum anderen ändert sich der mittlere Stufenabstand innerhalb der Cu-Streifen. Die hierbei gewonnenen Ergebnisse können im Vergleich mit den Ergebnissen diskutiert werden, die an den sauberen vizinalen Oberflächen gewonnen wurden. Mit größer werdender Bedeckung bildet sich ein neuer Zustand, dessen Ursprung in den Ag-Streifen liegt. Die beiden Zustände können in ihrer energetischen Lage und in ihrem Dispersionsverhalten unterschieden werden.
58

Theoretical studies of topology and strong correlations in superconductors

Hazra, Tamaghna January 2020 (has links)
No description available.
59

Effets d'une brisure de symétrie sur les stuctures électroniques d'URu2Si2 et de KTaO3

Bareille, Cédric 19 December 2013 (has links) (PDF)
L'étude des symétries d'un système peut en révéler de nombreuses propriétés physiques. La brisure, spontanée ou non, d'une de ces symétries implique alors d'importantes conséquences sur le comportement du système. On le voit dans la description actuelle de la physique des particules, avec notamment la création de la masse, ou dans la physique des solides, domaine de cette thèse, avec l'apparition de phases aux propriétés diverses, comme le magnétisme ou la supraconductivité. Le présent travail étudie par spectroscopie de photoémission résolue en angle (ARPES) les effets d'une brisure de symétrie dans deux systèmes différents : le système de fermions lourds URu2Si2 et l'oxyde de métal de transition (TMO) KTaO3. Le cristal d'URu2Si2 passe d'une phase paramagnétique pour T>THO, sujette à la cohérence de Kondo, vers la phase dite d'ordre caché pour T
60

Effets d'une brisure de symétrie sur les stuctures électroniques d'URu2Si2 et de KTaO3

Bareille, Cédric 19 December 2013 (has links) (PDF)
L'étude des symétries d'un système peut en révéler de nombreuses propriétés physiques. La brisure, spontanée ou non, d'une de ces symétries implique alors d'importantes conséquences sur le comportement du système. On le voit dans la description actuelle de la physique des particules, avec notamment la création de la masse, ou dans la physique des solides, domaine de cette thèse, avec l'apparition de phases aux propriétés diverses, comme le magnétisme ou la supraconductivité. Le présent travail étudie par spectroscopie de photoémission résolue en angle (ARPES) les effets d'une brisure de symétrie dans deux systèmes différents : le système de fermions lourds URu2Si2 et l'oxyde de métal de transition (TMO) KTaO3. Le cristal d'URu2Si2 passe d'une phase paramagnétique pour T>THO, sujette à la cohérence de Kondo, vers la phase dite d'ordre caché pour T

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