Equilibrium structure and shape of Ag and Pt nanoparticles grown on silica surfaces: from experimental investigations to the determination of a metal-silica potential

A combination of experimental and numerical calculations on metallic silver and platinum nanoparticles deposited on silica substrates is presented, with a focus on the metal-substrate interactions. Experimentally, the nanoparticles are elaborated under ultra-high vacuum and characterized by Grazing-Incidence Small-Angle X-ray Scattering (GISAXS) and High Resolution Transmission Electronic Microscopy (HRTEM) to determine their structure and morphology, and in particular their aspect ratio (height/diameter) which quantifies the metal-substrate interaction. Numerically, the interactions between the metal and the silica species are modeled with the Lennard-Jones (12, 6) potential, with two parameters for each metal and silica species. The geometric parameters were found in the literature, while the energetic parameters were determined from our experimental measurements of the aspect ratio. The parameters are: {\sigma}_{Ag-O} = 0.278 nm, {\sigma}_{Ag-Si} = 0.329 nm, {\epsilon}_{Ag-O} = 75 meV, and {\epsilon}_{Ag-Si} = 13 meV for Ag-silica and {\sigma}_{Pt-O} = 0.273 nm, {\sigma}_{Pt-Si} = 0.324 nm, {\epsilon}_{Pt-O} = 110 meV, and {\epsilon}_{Pt-Si} = 18 meV for Pt-silica. The proposed Ag-silica potential reproduces quantitatively the unexpected experimental observation of the variation of the aspect ratio for Ag nanoparticles larger than 5 nm, which has been interpreted as a consequence of the silica roughness. The nanoparticle orientation, structure and disorder are also considered. This metal-silica potential for Ag and Pt should be helpful for further studies on pure metals as well as their alloys.Comment: 35p, 12 figure

Fermi liquid behavior of the in-plane resistivity in the pseudogap state of YBa_2Cu_4O_8

Our knowledge of the ground state of underdoped hole-doped cuprates has evolved considerably over the last few years. There is now compelling evidence that inside the pseudogap phase, charge order breaks translational symmetry leading to a reconstructed Fermi surface made of small pockets. Quantum oscillations, [Doiron-Leyraud N, et al. (2007) Nature 447:564-568], optical conductivity [Mirzaei SI, et al. (2013) Proc Natl Acad Sci USA 110:5774-5778] and the validity of Wiedemann-Franz law [Grissonnache G, et al. (2016) Phys. Rev. B 93:064513] point to a Fermi liquid regime at low temperature in the underdoped regime. However, the observation of a quadratic temperature dependence in the electrical resistivity at low temperatures, the hallmark of a Fermi liquid regime, is still missing. Here, we report magnetoresistance measurements in the magnetic-field-induced normal state of underdoped YBa_2Cu_4O_8 which are consistent with a T^2 resistivity extending down to 1.5 K. The magnitude of the T^2 coefficient, however, is much smaller than expected for a single pocket of the mass and size observed in quantum oscillations, implying that the reconstructed Fermi surface must consist of at least one additional pocket.Comment: Main + SI : published versio

Correlation between Fermi surface transformations and superconductivity in the electron-doped high-TcT_c superconductor Nd2−x_{2-x}Cex_xCuO4_4

Two critical points have been revealed in the normal-state phase diagram of the electron-doped cuprate superconductor Nd$_{2-x}$Ce$_x$CuO$_4$ by exploring the Fermi surface properties of high quality single crystals by high-field magnetotransport. First, the quantitative analysis of the Shubnikov-de Haas effect shows that the weak superlattice potential responsible for the Fermi surface reconstruction in the overdoped regime extrapolates to zero at the doping level $x_c = 0.175$ corresponding to the onset of superconductivity. Second, the high-field Hall coefficient exhibits a sharp drop right below optimal doping $x_{\mathrm{opt}} = 0.145$ where the superconducting transition temperature is maximum. This drop is most likely caused by the onset of long-range antiferromagnetic ordering. Thus, the superconducting dome appears to be pinned by two critical points to the normal state phase diagram.Comment: 9 pages; 7 figures; 1 tabl

Universal magnetic structure of the half-magnetization phase in Cr-based spinels

Using an elastic neutron scattering technique under a pulsed magnetic field up to 30 T, we determined the magnetic structure in the half-magnetization plateau phase in the spinel CdCr$_2$O$_4$. The magnetic structure has a cubic $P4_3$32 symmetry, which is the same as that observed in HgCr$_2$O$_4$. This suggests that there is a universal field induced spin-lattice coupling mechanism at work in the Cr-based spinels.Comment: 4 pages, 4 figure

Shubnikov-de Haas oscillations in YBa_2Cu_4O_8

We report the observation of Shubnikov-de Haas oscillations in the underdoped cuprate superconductor YBa$_2$Cu$_4$O$_8$ (Y124). For field aligned along the c-axis, the frequency of the oscillations is $660\pm 30$ T, which corresponds to $\sim 2.4$ % of the total area of the first Brillouin zone. The effective mass of the quasiparticles on this orbit is measured to be $2.7\pm0.3$ times the free electron mass. Both the frequency and mass are comparable to those recently observed for ortho-II YBa$_2$Cu$_3$O$_{6.5}$ (Y123-II). We show that although small Fermi surface pockets may be expected from band structure calculations in Y123-II, no such pockets are predicted for Y124. Our results therefore imply that these small pockets are a generic feature of the copper oxide plane in underdoped cuprates.Comment: v2: Version of paper accepted for publication in Physical Review Letters. Only minor changes to the text and reference

Angle-dependence of quantum oscillations in YBa2Cu3O6.59 shows free spin behaviour of quasiparticles

Measurements of quantum oscillations in the cuprate superconductors afford a new opportunity to assess the extent to which the electronic properties of these materials yield to a description rooted in Fermi liquid theory. However, such an analysis is hampered by the small number of oscillatory periods observed. Here we employ a genetic algorithm to globally model the field, angular, and temperature dependence of the quantum oscillations observed in the resistivity of YBa2Cu3O6.59. This approach successfully fits an entire data set to a Fermi surface comprised of two small, quasi-2-dimensional cylinders. A key feature of the data is the first identification of the effect of Zeeman splitting, which separates spin-up and spin-down contributions, indicating that the quasiparticles in the cuprates behave as nearly free spins, constraining the source of the Fermi surface reconstruction to something other than a conventional spin density wave with moments parallel to the CuO2 planes.Comment: 8 pages, 4 figure

Lifshitz critical point in the cuprate superconductor YBa2Cu3Oy from high-field Hall effect measurements

The Hall coefficient R_H of the cuprate superconductor YBa2Cu3Oy was measured in magnetic fields up to 60 T for a hole concentration p from 0.078 to 0.152, in the underdoped regime. In fields large enough to suppress superconductivity, R_H(T) is seen to go from positive at high temperature to negative at low temperature, for p > 0.08. This change of sign is attributed to the emergence of an electron pocket in the Fermi surface at low temperature. At p < 0.08, the normal-state R_H(T) remains positive at all temperatures, increasing monotonically as T \to 0. We attribute the change of behaviour across p = 0.08 to a Lifshitz transition, namely a change in Fermi-surface topology occurring at a critical concentration p_L = 0.08, where the electron pocket vanishes. The loss of the high-mobility electron pocket across p_L coincides with a ten-fold drop in the conductivity at low temperature, revealed in measurements of the electrical resistivity $\rho$ at high fields, showing that the so-called metal-insulator crossover of cuprates is in fact driven by a Lifshitz transition. It also coincides with a jump in the in-plane anisotropy of $\rho$, showing that without its electron pocket the Fermi surface must have strong two-fold in-plane anisotropy. These findings are consistent with a Fermi-surface reconstruction caused by a unidirectional spin-density wave or stripe order.Comment: 16 pages, 13 figures, see associated Viewpoint: M. Vojta, Physics 4, 12 (2011

Evidence for a small hole pocket in the Fermi surface of underdoped YBa2Cu3Oy

The Fermi surface of a metal is the fundamental basis from which its properties can be understood. In underdoped cuprate superconductors, the Fermi surface undergoes a reconstruction that produces a small electron pocket, but whether there is another, as yet undetected portion to the Fermi surface is unknown. Establishing the complete topology of the Fermi surface is key to identifying the mechanism responsible for its reconstruction. Here we report the discovery of a second Fermi pocket in underdoped YBa2Cu3Oy, detected as a small quantum oscillation frequency in the thermoelectric response and in the c-axis resistance. The field-angle dependence of the frequency demonstrates that it is a distinct Fermi surface and the normal-state thermopower requires it to be a hole pocket. A Fermi surface consisting of one electron pocket and two hole pockets with the measured areas and masses is consistent with a Fermi-surface reconstruction caused by the charge-density-wave order observed in YBa2Cu3Oy, provided other parts of the reconstructed Fermi surface are removed by a separate mechanism, possibly the pseudogap.Comment: 23 pages, 5 figure

Hall, Seebeck, and Nernst Coefficients of Underdoped HgBa2CuO4+d: Fermi-Surface Reconstruction in an Archetypal Cuprate Superconductor

Charge density-wave order has been observed in cuprate superconductors whose crystal structure breaks the square symmetry of the CuO2 planes, such as orthorhombic YBa2Cu3Oy (YBCO), but not so far in cuprates that preserve that symmetry, such as tetragonal HgBa2CuO4+d (Hg1201). We have measured the Hall (R_H), Seebeck (S), and Nernst coefficients of underdoped Hg1201 in magnetic fields large enough to suppress superconductivity. The high-field R_H(T) and S(T) are found to drop with decreasing temperature and become negative, as also observed in YBCO at comparable doping. In YBCO, the negative R_H and S are signatures of a small electron pocket caused by Fermi-surface reconstruction, attributed to charge density-wave modulations observed in the same range of doping and temperature. We deduce that a similar Fermi-surface reconstruction takes place in Hg1201, evidence that density-wave order exists in this material. A striking similarity is also found in the normal-state Nernst coefficient, further supporting this interpretation. Given the model nature of Hg1201, Fermi-surface reconstruction appears to be common to all hole-doped cuprates, suggesting that density-wave order is a fundamental property of these materials