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1.
Proc Natl Acad Sci U S A ; 120(36): e2307334120, 2023 Sep 05.
Article in English | MEDLINE | ID: mdl-37639594

ABSTRACT

The layered delafossite metal PdCrO[Formula: see text] is a natural heterostructure of highly conductive Pd layers Kondo coupled to localized spins in the adjacent Mott insulating CrO[Formula: see text] layers. At high temperatures, T, it has a T-linear resistivity which is not seen in the isostructural but nonmagnetic PdCoO[Formula: see text]. The strength of the Kondo coupling is known, as-grown crystals are extremely high purity and the Fermi surface is both very simple and experimentally known. It is therefore an ideal material platform in which to investigate "Planckian metal" physics. We do this by means of controlled introduction of point disorder, measurement of the thermal conductivity and Lorenz ratio, and studying the sources of its high-temperature entropy. The T-linear resistivity is seen to be due mainly to elastic scattering and to arise from a sum of several scattering mechanisms. Remarkably, this sum leads to a scattering rate within 10[Formula: see text] of the Planckian value of k[Formula: see text]T/[Formula: see text].

2.
Sci Technol Adv Mater ; 22(1): 583-596, 2021.
Article in English | MEDLINE | ID: mdl-34377085

ABSTRACT

The interplay between charges and spins may influence the dynamics of the carriers and determine their thermoelectric properties. In that respect, magneto-thermoelectric power MTEP, i.e. the measurements of the Seebeck coefficient S under the application of an external magnetic field, is a powerful technique to reveal the role of magnetic moments on S. This is illustrated by different transition metal chalcogenides: CuCrTiS4 and CuMnTiS4 magnetic thiospinels, which are compared with magnetic oxides, Curie-Weiss (CW) paramagnetic misfit cobaltites, ruthenates, either ferromagnetic perovskite or Pauli paramagnet quadruple perovskites, and CuGa1-x Mn x Te2 chalcopyrite telluride and Bi1.99Cr0.01Te3 in which diluted magnetism is induced by 3%-Mn and 1%-Cr substitution, respectively. In the case of a ferromagnet (below TC) and CW paramagnetic materials, the increase of magnetization at low T when a magnetic field is applied is accompanied by a decrease of the entropy of the carriers and hence S decreases. This is consistent with the lack of MTEP in the Pauli paramagnetic quadruple perovskites. Also, no significant MTEP is observed in CuGa1-x Mn x Te2 and Bi1.99Cr0.01Te3, for which Kondo-type interaction between magnetic moments and carriers prevails. In contrast, spin glass CuCrTiS4 exhibits negative MTEP like in ferromagnetic ruthenates and paramagnetic misfit cobaltites. This investigation of some chalcogenides and oxides provides key ingredients to select magnetic materials for which S benefits from spin entropy.

3.
Science ; 373(6558): 1017-1022, 2021 08 27.
Article in English | MEDLINE | ID: mdl-34446603

ABSTRACT

The thermal conductivity of crystalline materials cannot be arbitrarily low, as the intrinsic limit depends on the phonon dispersion. We used complementary strategies to suppress the contribution of the longitudinal and transverse phonons to heat transport in layered materials that contain different types of intrinsic chemical interfaces. BiOCl and Bi2O2Se encapsulate these design principles for longitudinal and transverse modes, respectively, and the bulk superlattice material Bi4O4SeCl2 combines these effects by ordering both interface types within its unit cell to reach an extremely low thermal conductivity of 0.1 watts per kelvin per meter at room temperature along its stacking direction. This value comes within a factor of four of the thermal conductivity of air. We demonstrated that chemical control of the spatial arrangement of distinct interfaces can synergically modify vibrational modes to minimize thermal conductivity.

4.
Rev Sci Instrum ; 90(2): 024902, 2019 Feb.
Article in English | MEDLINE | ID: mdl-30831733

ABSTRACT

We present a simplified, rapid, and accurate method for the measurement of the thermoelectric Thomson coefficient by the dynamical heating of a suspended wire by an alternating current. By applying a temperature gradient across the wire, we find that the response at the second harmonic of the excitation frequency is directly proportional to the Thomson coefficient. The absolute thermoelectric coefficient of a single material can therefore be extracted with high precision by using a phase sensitive detector. We test our method on platinum and nickel wires and develop both analytical and numerical models to determine the leading sources of error.

5.
J Am Chem Soc ; 140(6): 2186-2195, 2018 02 14.
Article in English | MEDLINE | ID: mdl-29332398

ABSTRACT

High-performance thermoelectric bulk sulfide with the colusite structure is achieved by controlling the densification process and forming short-to-medium range structural defects. A simple and powerful way to adjust carrier concentration combined with enhanced phonon scattering through point defects and disordered regions is described. By combining experiments with band structure and phonons calculations, we elucidate, for the first time, the underlying mechanism at the origin of intrinsically low thermal conductivity in colusite samples as well as the effect of S vacancies and antisite defects on the carrier concentration. Our approach provides a controlled and scalable method to engineer high power factors and remarkable figures of merit near the unity in complex bulk sulfide such as Cu26V2Sn6S32 colusites.

6.
Sensors (Basel) ; 17(11)2017 Nov 08.
Article in English | MEDLINE | ID: mdl-29117137

ABSTRACT

In this work, we review single mode SiO2 fiber Bragg grating techniques for dilatometry studies of small single-crystalline samples in the extreme environments of very high, continuous, and pulsed magnetic fields of up to 150 T and at cryogenic temperatures down to <1 K. Distinct millimeter-long materials are measured as part of the technique development, including metallic, insulating, and radioactive compounds. Experimental strategies are discussed for the observation and analysis of the related thermal expansion and magnetostriction of materials, which can achieve a strain sensitivity (ΔL/L) as low as a few parts in one hundred million (≈10-8). The impact of experimental artifacts, such as those originating in the temperature dependence of the fiber's index of diffraction, light polarization rotation in magnetic fields, and reduced strain transfer from millimeter-long specimens, is analyzed quantitatively using analytic models available in the literature. We compare the experimental results with model predictions in the small-sample limit, and discuss the uncovered discrepancies.

7.
J Phys Condens Matter ; 29(7): 075604, 2017 Feb 22.
Article in English | MEDLINE | ID: mdl-28035090

ABSTRACT

The chalcogenide superconductor Rh17S15 is known for having an upper critical field of nearly twice the Pauli limit and an unusual temperature dependence of the resistivity. When doped with small amounts of cobalt, superconductivity in Rh17-x Co x S15 (0 < x < 3) is systematically suppressed. We explore the evolution of the electrical transport properties from 2-300 K as a function of x. We identify three temperature regimes which are differently affected by doping. The disappearance of an electron-like contribution to the transport at low temperature is correlated with the suppression of superconductivity.

8.
Sci Technol Adv Mater ; 18(1): 919-938, 2017.
Article in English | MEDLINE | ID: mdl-29383043

ABSTRACT

The electronic transport properties of the delafossite oxides [Formula: see text] are usually understood in terms of two well-separated entities, namely the triangular [Formula: see text] and ([Formula: see text] layers. Here, we review several cases among this extensive family of materials where the transport depends on the interlayer coupling and displays unconventional properties. We review the doped thermoelectrics based on [Formula: see text] and [Formula: see text], which show a high-temperature recovery of Fermi-liquid transport exponents, as well as the highly anisotropic metals [Formula: see text], [Formula: see text], and [Formula: see text], where the sheer simplicity of the Fermi surface leads to unconventional transport. We present some of the theoretical tools that have been used to investigate these transport properties and review what can and cannot be learned from the extensive set of electronic structure calculations that have been performed.

9.
Rev Sci Instrum ; 81(3): 033909, 2010 Mar.
Article in English | MEDLINE | ID: mdl-20370194

ABSTRACT

We report on a new high resolution apparatus for measuring magnetostriction suitable for use at cryogenic temperatures in pulsed high magnetic fields which we have developed at the Hochfeld-Magnetlabor Dresden. Optical fiber strain gauges based on fiber Bragg gratings are used to measure the strain in small (approximately 1 mm) samples. We describe the implementation of a fast measurement system capable of resolving strains in the order of 10(-7) with a full bandwidth of 47 kHz, and demonstrate its use on single crystal samples of GdSb and GdSi.

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