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S. Hebert

Publications and source records attributed to S. Hebert.

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High-throughput synthesis of thermoelectric Ca$_3$Co$_4$O$_9$ films

Properties of complex oxide thin films can be tuned over a range of values as a function of mismatch, composition, orientation, and structure. Here, we report a strategy for growing structured epitaxial thermoelectric thin films leading to improved Seebeck coefficient. Instead of using single-crystal sapphire substrates to support epitaxial growth, Ca$_3$Co$_4$O$_9$ films are deposited, using the Pulsed Laser Deposition technique, onto Al$_2$O$_3$ polycrystalline substrates textured by Spark Plasma Sintering. The structural quality of the 2000 \AA thin film was investigated by Transmission Electron Microscopy, while the crystallographic orientation of the grains and the epitaxial relationships were determined by Electron Back Scatter Diffraction. The use of a polycrystalline ceramic template leads to structured films that are in good local epitaxial registry. The Seebeck coefficient is about 170 $\mu$V/K at 300 K, a typical value of misfit material with low carrier density. This high-throughput process, called combinatorial substrate epitaxy, appears to facilitate the rational tuning of functional oxide films, opening a route to the epitaxial synthesis of high quality complex oxides.

cond-mat.mtrl-sci

Magnetic field dependent specific heat and enhanced Wilson ratio in strongly correlated layered cobalt oxide

We have investigated the low temperature specific heat properties as a function of magnetic field in the strongly correlated layered cobalt oxide [BiBa$_{0.66}$K$_{0.36}$O$_2$]CoO$_2$. These measurements reveal two kinds of magnetic field dependent contributions in qualitative agreement with the presence of a previously inferred magnetic Quantum Critical Point (QCP). First, the coefficient of the low temperature T$^3$ behavior of the specific heat turns out to sizeably decrease near a magnetic field consistent with the critical value reported in a recent paper. In addition, a moderate but significant enhancement of the Sommerfeld coefficient is found in the vicinity of the QCP suggesting a slight increase of the electronic effective mass. This result contrasts with the divergent behavior of the previously reported Pauli susceptibility. Thus, a strongly enhanced Wilson ratio is deduced, suggesting efficient ferromagnetic fluctuations in the Fermi liquid regime which could explain the unusual magnetic field dependent specific heat. As a strong check, the high magnetic field Wilson ratio asymptotically recovers the universal limit of the local Fermi liquid against ferromagnetism.

cond-mat.str-el

Transport and magnetic properties in YBaCo2O5.45: Focus on the high-temperature transition

The electronic transport properties and the magnetic susceptibility were measured in detail in $YBaCo_2O_{5.45}$. Close to the so-called metal-insulator transition, strong effects of resistance relaxation, a clear thermal hysteresis and a sudden increase of the resistance noise are observed. This is likely due to the first order character of the transition and to the underlying phases coexistence. Despite these out of equilibrium features, a positive and linear magneto-resistance is also observed, possibly linked to the heterogeneity of the state. From a magnetic point of view, the paramagnetic to ordered magnetic state transition is observed using non linear susceptibilty. This transition shows the characteristics of a continuous transition, and time dependent effects can be linked with the dynamics of magnetic domains in presence of disorder. Thus, when focusing on the order of the transitions, the electronic one and the magnetic one can not be directly associated.

cond-mat.mtrl-sci

Interplay between magnetic properties and thermoelectricity in misfit and Na cobaltates

We present a comparative study of CoO2 layers in the Bi-misfit and NaxCoO2 cobaltates. Co NMR measures the intrinsic susceptibility of the Co layers and is not affected by spurious contributions. At low dopings where room-temperature thermopower (TEP) is large, Curie-Weiss susceptibilities are observed in both materials. But NMR and muSR experiments find neither charge nor spin order down to low temperatures in Bi-misfit, in contrast to the case of NaxCoO2. This demonstrates that metallicity, charge and magnetic orders are specific of the Na layers in NaxCoO2 whereas strong correlations are generic of the cobaltates physics and could explain the large TEP.

cond-mat.str-el

Direct observation of strong correlations near the band insulator regime of Bi misfit cobaltates

We present the first angle-resolved photoemission (ARPES) measurement of Fermi Surface in the "misfit" cobaltate [Bi2Ba2O4].[CoO2]~2. This compound contains the same triangular Co planes as Na cobaltates, but in a different 3D environment. Our data establish the similarity of their electronic structure. We propose that the peculiar lineshape of all cobaltates is of the "peak-dip-hump" type, due to strong many-body effects. We detect a progressive transfer of spectral weight from the quasiparticle feature near Ef to a broad hump in misfit phases where Ba is replaced by Sr or Ca. This indicates stronger many-body interactions in proximity of the band insulator regime, which we attribute to the presence of unusual magnetic excitations.

cond-mat.str-el

Electronic Correlations in CoO2, the Parent Compound of Triangular Cobaltates

A 59Co NMR study of CoO2, the x=0 end member of AxCoO2 (A = Na, Li...) cobaltates, reveals a metallic ground state, though with clear signs of strong electron correlations: low-energy spin fluctuations develop at wave vectors q different from 0 and a crossover to a Fermi-liquid regime occurs below a characteristic temperature T*~7 K. Despite some uncertainty over the exact cobalt oxidation state n this material, the results show that electronic correlations are revealed as x is reduced below 0.3. The data are consistent with NaxCoO2 being close to the Mott transition in the x -> 0 limit.

cond-mat.str-el

Metastable diamagnetism in Sm0.1Ca0.84Sr0.06MnO3 manganite

Magnetic properties of polycrystalline Sm0.1Ca0.84Sr0.06MnO3 in pristine and metastable states have been investigated in wide range of temperatures and magnetic fields. It was found that below Curie temperature TC = 105 K the pristine state exhibits phase separation comprising ferromagnetic and antiferromagnetic phases. The metastable states with reduced magnetization were obtained by successive number of quick coolings of the sample placed in container with kerosene-oil mixture. By an increasing number of quick coolings (> 6) the long time relaxation appeared at 10 K and the magnetization reversed its sign and became strongly negative in wide temperature range, even under an applied magnetic field of 15 kOe. The observed field and temperature dependences of the magnetization in this state are reversed in comparison with the ordinary ferromagnetic ones. Above TC, the observed diamagnetic susceptibility of the reversed magnetization state at T = 120 K is ~ - 0.9 x 10-4 emu g-1 Oe-1. Only after some storage time at room temperature, the abnormal magnetic state is erasable. It is suggested that the negative magnetization observed results from a specific coupling of the nano/micro-size ferromagnetic regions with a surrounding diamagnetic matrix formed, in a puzzled way, by the repeating training (quick cooling) cycles.

cond-mat.str-el

Scaling behavior in thermoelectric misfit cobalt oxides

We investigate both thermoelectric and thermodynamic properties of the misfit cobalt oxide [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$. A large negative magnetothermopower is found to scale with both magnetic field and temperature revealing a significant spin entropy contribution to thermoelectric properties giving rise to a constant S$_0\approx$ 60 $μ$V K$^{-1}$ equal to the high temperature asymptotic value of the spin 1/2 entropy. Low temperature specific heat measurements allow us to determine an enhanced electronic part with $γ\approx$ 50 mJ (mol K$^{2}$)$^{-1}$ attesting of strong correlations. Thereby, a critical comparison between [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$, other cobaltites as well as other materials reveals a universal behavior of the thermopower low temperature slope as a function of $γ$ testifying thus a purely electronic origin. This potentially generic scaling behavior suggests here that the high room temperature value of the thermopower in misfit cobalt oxides results from the addition of a spin entropy contribution to an enlarged electronic one.

cond-mat.str-el

Strongly correlated properties of the thermoelectric cobalt oxide Ca3Co4O9

We have performed both in-plane resistivity, Hall effect and specific heat measurements on the thermoelectric cobalt oxide Ca$_{3}$Co$_{4}$O$_{9}$. Four distinct transport regimes are found as a function of temperature, corresponding to a low temperature insulating one up to $T_{min}\approx $63 K, a strongly correlated Fermi liquid up to $T^*\approx $140 K, with $ρ=ρ_0+AT^2$ and $A\approx 3.63$ $10^{-2} μΩcm/K^{2}$, followed by an incoherent metal with $k_Fl\leq 1$ and a high temperature insulator above T$^{**}\approx $510 K . Specific heat Sommerfeld coefficient $γ= 93$ mJ/(mol.K$^{2}$) confirms a rather large value of the electronic effective mass and fulfils the Kadowaki-Woods ratio $A/γ^2 \approx 0.45$ 10$^{-5}$ $μΩcm.K^2/(mJ^2mol^{-2})$. Resistivity measurements under pressure reveal a decrease of the Fermi liquid transport coefficient A with an increase of $T^*$ as a function of pressure while the product $A(T^*)^2/a$ remains constant and of order $h/e^2$. Both thermodynamic and transport properties suggest a strong renormalization of the quasiparticles coherence scale of order $T^*$ that seems to govern also thermopower.

cond-mat.str-el

Quantum Tunneling of the Magnetization in the Ising Chain Compound Ca3Co2O6

The magnetic behavior of the Ca3Co2O6 spin chain compound is characterized by a large Ising-like character of its ferromagnetic chains, set on triangular lattice, that are antiferromagnetically coupled. At low temperature, T < 7K, the 3D antiferromagnetic state evolves towards a spin frozen state. In this temperature range, magnetic field driven magnetization of single crystals (H//chains) exhibits stepped variations. The occurrence of these steps at regular intervals of the applied magnetic field, Hstep=1.2T, is reminiscent of the quantum tunneling of the magnetization (QTM) of molecular based magnets. Magnetization relaxation experiments also strongly support the occurrence of this quantum phenomenon. This first observation of QTM in a magnetic oxide belonging to the large family of the A3BBO6 compounds opens new opportunities to study a quantum effect in a very different class of materials from molecular magnets.

cond-mat.str-el

Dome-shaped magnetic phase diagram of thermoelectric layered cobaltites

Using muon spin spectroscopy we have found that, for both Na$_x$CoO$_2$ (0.6 $\leq x \leq$ 0.9) and 3- and 4-layer cobaltites, a common low temperature magnetic state (which in some cases is manifest as an incommensurate spin density wave) forms in the CoO$_2$ planes. Here we summarize those results and report a dome-shaped relation between the transition temperature into the low-$T$ magnetic state and the composition $x$ for Na$_x$CoO$_2$ and/or the high-temperature asymptotic limit of thermopower in the more complex 3- and 4-layer cobaltites. This behavior is explained using the Hubbard model on two-dimensional triangular lattice in the CoO$_2$ plane.

cond-mat.str-el

Neutron scattering evidence for magnetic field driven abrupt magnetic and structural transitions in a phase separated manganite

Substitutions at the Mn-site of the charge-ordered Pr0.5Ca0.5MnO3 manganite is an effective way to induce abrupt jumps on the magnetic field driven magnetization curve. In order to get new insights into the origin of this remarkable feature, the Pr0.5Ca0.5Mn0.97Ga0.03O3 perovskite manganite has been studied by neutron diffraction, versus temperature and at 2.5K in an applied magnetic field up to 6 Tesla. A weak and complex antiferromagnetic order is found for the low temperature ground-state. Magnetic transitions, associated with structural ones, are evidenced for certain strengths of magnetic field, which gives rise to the step-like behavior corresponding to the magnetization curve. Small angle neutron scattering provides evidence for a nucleation process of micron size ferromagnetic domains which follows the magnetization behavior.

cond-mat.mtrl-sci

Field-Induced Magnetization Steps in Intermetallic Compounds and Manganese Oxides: The Martensitic Scenario

Field-induced magnetization jumps with similar characteristics are observed at low temperature for the intermetallic germanide Gd5Ge4and the mixed-valent manganite Pr0.6Ca0.4Mn0.96Ga0.04O3. We report that the field location -and even the existence- of these jumps depends critically on the magnetic field sweep rate used to record the data. It is proposed that, for both compounds, the martensitic character of their antiferromagnetic-to-ferromagnetic transitions is at the origin of the magnetization steps.

cond-mat.mtrl-sci

Staircase-like metamagnetic transitions in phase-separated manganites: influence of thermal and mechanical treatments

Substitutions in the Mn-sublattice of antiferromagnetic, charge and orbitally ordered manganites was recently found to produce intriguing metamagnetic transitions, consisting of a succession of sharp magnetization steps separated by plateaus. The compounds exhibiting such features can be divided in two categories, depending on whether they are sensitive to thermal cycling effects or not. One compound of each category has been considered in the present study. The paper reports on the influence of two treatments: high-temperature annealing and grinding. It is shown that both of these treatments can drastically affect the phenomenon of magnetization steps. These results provide us with new information about the origin of these jumps in magnetization.

cond-mat.mtrl-sci

Specific heat investigation of the magnetic ordering in two frustrated spin-chain oxides: Ca3Co2O6 and Ca3CoRhO6

Specific heat measurements were carried out on the closely related spin-chain oxides Ca3Co2O6 and Ca3CoRhO6. Both compounds consist of Ising magnetic chains that are arranged on a triangular lattice. The spin coupling along and between the chains are ferromagnetic and antiferromagnetic, respectively. Geometrical frustration is expected from the combination of these magnetic features. The present study reports that the specific heat data of these compounds exhibit similarities in the spin-freezing process at low T, whereas striking differences exist in the antiferromagnetic interchain ordering at higher T. These results are discussed in connection with previous magnetization and neutron diffraction data.

cond-mat.str-el

Staircase effect in metamagnetic transitions of charge and orbitally ordered manganites

This paper reports on peculiar metamagnetic transitions which take place in antiferromagnetic, charge and orbitally ordered (AFCOO) manganites. At very low temperatures, the virgin magnetization curves of some of these compounds exhibit several, sharp steps giving rise to a staircase-like shape. This staircase effect is shown to be sensitive to various experimental parameters. Several potential interpretations of the staircase effect are discussed in relation to this set of results. A martensitic-like scenario, involving a leading role of the structural distortions associated to the collapse of the orbital ordering, is found to be the most plausible interpretation.

cond-mat.str-el

Ultra-sharp magnetization steps in perovskite manganites

We report a detailed study of step-like metamagnetic transitions in the magnetization and resistivity of polycrystalline Pr0.5Ca0.5Mn0.95Co0.05O3. The steps have a sudden onset below a critical temperature, are extremely sharp (width < 0.2 mT), and occur at critical fields which are linearly dependent on the absolute value of the cooling field in which the sample is prepared. Similar transitions are also observed at low temperature in non-Co doped manganites, including single crystal samples. These data show that the steps are an intrinsic property, qualitatively different from either previously observed higher temperature metamagnetic transitions in the manganites or metamagnetic transitions observed in other materials.

cond-mat.mtrl-sci