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1.
Phys Rev Lett ; 117(21): 216401, 2016 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-27911533

RESUMO

The "failed Kondo insulator" CeNiSn has long been suspected to be a nodal metal, with a node in the hybridization matrix elements. Here we carry out a series of Nernst effect experiments to delineate whether the severely anisotropic magnetotransport coefficients do indeed derive from a nodal metal or can simply be explained by a highly anisotropic Fermi surface. Our experiments reveal that despite an almost twentyfold anisotropy in the Hall conductivity, the large Nernst signal is isotropic. Taken in conjunction with the magnetotransport anisotropy, these results provide strong support for an isotropic Fermi surface with a large anisotropy in quasiparticle mass derived from a nodal hybridization.

2.
Inorg Chem ; 51(21): 11396-405, 2012 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-23072375

RESUMO

The new cationic clathrates I Si(30)P(16)Te(8-x)Se(x) and Si(30+x)P(16-x)Te(8-x)Br(x) were synthesized by the standard ampule technique. The Si(30)P(16)Te(8-x)Se(x) (x = 0-2.3) clathrates crystallize in the cubic space group Pm3̅n with the unit cell parameter a ranging from 9.9382(2) to 9.9696(1) Å. In the case of the Si(30+x)P(16-x)Te(8-x)Br(x) (x = 1-6.4) clathrates, the lattice parameter varies from 9.9720(8) to 10.0405(1) Å; at lower Si/P ratios (x = 1-3) the ordering of bromine atoms induces the splitting of the guest positions and causes the transformation from the space group Pm3n to Pm3. Irrespective of the structure peculiarities, the normal temperature motion of the guest atoms inside the oversized cages of the framework is observed. The title clathrates possess very low thermal expansion coefficients ranging from 6.6 × 10(-6) to 1.0 × 10(-5) K(-1) in the temperature range of 298-1100 K. The characteristic Debye temperature is about 490 K. Measurements of the electrical resistivity and thermopower showed typical behavior of p-type thermally activated semiconductors, whereas the temperature behavior of the thermal conductivity is glasslike and in general consistent with the PGEC concept. The highest value of the thermoelectric figure of merit (ZT = 0.1) was achieved for the Br-bearing clathrate Si(32.1(2))P(13.9(2))Te(6.6(2))Br(1.0(1)) at 750 K.

3.
Phys Rev Lett ; 108(6): 066405, 2012 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-22401095

RESUMO

Thermodynamic and transport properties of the La-diluted Kondo lattice CeNi(2)Ge(2) were studied in a wide temperature range. The Ce-rich alloys Ce(1-x)La(x)Ni(2)Ge(2) were found to exhibit distinct features of the coherent heavy Fermi liquid. At intermediate compositions (0.7≤x≤0.9), non-Fermi liquid properties have been observed, followed by the local Fermi liquid behavior in the dilute limit. The 4f-electron contribution to the specific heat was found to follow the predictions of the Kondo-impurity model in both the local as well as the coherent regimes, with the characteristic Kondo temperature decreasing rapidly from about 30 K for the parent compound CeNi(2)Ge(2) to about 1 K in the most dilute samples. The specific heat does not show any evidence for the emergence of a new characteristic energy scale related to the formation of the coherent Kondo lattice.

4.
ACS Nano ; 5(11): 8541-51, 2011 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-21981245

RESUMO

We present the full thermoelectric characterization of nanostructured bulk PbTe and PbTe-PbSe samples fabricated from colloidal core-shell nanoparticles followed by spark plasma sintering. An unusually large thermopower is found in both materials, and the possibility of energy filtering as opposed to grain boundary scattering as an explanation is discussed. A decreased Debye temperature and an increased molar specific heat are in accordance with recent predictions for nanostructured materials. On the basis of these results we propose suitable core-shell material combinations for future thermoelectric materials of large electric conductivities in combination with an increased thermopower by energy filtering.

5.
ACS Nano ; 5(11): 9052-61, 2011 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-21978378

RESUMO

Engineering nanoscale interfaces is a requisite for harnessing electrical and thermal transports within nanostructured materials, especially those destined for thermoelectric applications requiring an unusual combination of low thermal conductivity and electrical resistivity. Nanocomposites open up possibilities in this area, but are still bound to a very narrow range of materials. Here, we report a new approach combining the sol-gel process toward hybrid materials with spark plasma sintering (SPS) to yield functional nanocomposites based on substoichiometric titanium oxides Ti(n)O(2n-1), so-called Magnéli phases. The potential of this new approach is demonstrated by three results. First, multiple Ti(n)O(2n-1) compounds (n = 3, 4, 5, 6, 8) are obtained for the first time as sole nano-Magnéli crystalline phases with controlled specific surface areas from 55 to 300 m(2)·g(-1), classified as potential thermoelectric n-type metal oxides and paving the way toward advanced systems for energy-harvesting devices and optoelectronics. Second, this work combines the use of sol-gel and SPS processes to yield percolated nanocomposites based on metal oxide nanoparticles embedded in a carbon matrix with low electrical resistivity (2 × 10(-4) Ω·m for a Ti(4)O(7) compound) and reduced thermal conductivity (1 W·m(-1)·K(-1)) with respect to bulk phases. Finally, the discovered materials are reliable with thermoelectric figures of merit (ZT = 0.08) relatively high for n-type Ti-O-based systems and metal oxides. Thereby this study represents a proof of concept for the development of promising, cheaper, and more efficient thermoelectric conversion devices.

6.
J Phys Condens Matter ; 23(9): 094216, 2011 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-21339569

RESUMO

YbRh2Si2 is a model system for quantum criticality. In particular, Hall effect measurements helped identify the unconventional nature of its quantum critical point. Here, we present a high-resolution study of the Hall effect and magnetoresistivity on samples of different quality. We find a robust crossover on top of a sample dependent linear background contribution. Our detailed analysis provides a complete characterization of the crossover in terms of its position, width, and height. Importantly, we find in the extrapolation to zero temperature a discontinuity of the Hall coefficient occurring at the quantum critical point for all samples. In particular, the height of the jump in the Hall coefficient remains finite in the limit of zero temperature. Hence, our data solidify the conclusion of a collapsing Fermi surface. Finally, we contrast our results to the smooth Hall effect evolution seen in chromium, the prototype system for a spin-density-wave quantum critical point.

7.
Inorg Chem ; 50(4): 1250-7, 2011 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-21250680

RESUMO

Single crystals of Ba(8)Au(5.3)Ge(40.7) [space group Pm(3)n (No. 223), a = 10.79891(8) Å] were prepared by a Bridgman technique. The crystal structure refinement based on single-crystal X-ray diffraction data does not reveal any vacancies in the Au/Ge framework or in the cages. In addition to the ionic bonding between Ba and the anionic framework, a direct interaction between Ba and Au atoms was identified in Ba(8)Au(5.3)Ge(40.7) by applying the electron localizability indicator. As expected by the chemical-bonding picture, Ba(8)Au(5.3)Ge(40.7) is a diamagnet and shows p-type electrical conductivity with a hole carrier concentration of 7.14 × 10(19) cm(-3) at 300 K and very low lattice thermal conductivity of ≈0.6 W m(-1) K(-1) at 500 K. The thermoelectric figure of merit ZT of single crystals of Ba(8)Au(5.3)Ge(40.7) attains 0.3 at 511 K and reaches 0.9 at 680 K in a polycrystalline sample of closely similar composition. This opens up an opportunity for tuning of the thermoelectric properties of materials in the Ba-Au-Ge clathrate system by changing the chemical composition.

8.
J Am Chem Soc ; 132(32): 10984-5, 2010 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-20698650

RESUMO

BaGe(5) constitutes a new type of intermetallic clathrate obtained by decomposition of clathrate-I Ba(8)Ge(43)(3) at low temperatures. The crystal structure consists of characteristic layers interconnected by covalent bonds. BaGe(5) is a semiconducting Zintl phase.

9.
Proc Natl Acad Sci U S A ; 107(33): 14547-51, 2010 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-20668246

RESUMO

Quantum criticality arises when a macroscopic phase of matter undergoes a continuous transformation at zero temperature. While the collective fluctuations at quantum-critical points are being increasingly recognized as playing an important role in a wide range of quantum materials, the nature of the underlying quantum-critical excitations remains poorly understood. Here we report in-depth measurements of the Hall effect in the heavy-fermion metal YbRh(2)Si(2), a prototypical system for quantum criticality. We isolate a rapid crossover of the isothermal Hall coefficient clearly connected to the quantum-critical point from a smooth background contribution; the latter exists away from the quantum-critical point and is detectable through our studies only over a wide range of magnetic field. Importantly, the width of the critical crossover is proportional to temperature, which violates the predictions of conventional theory and is instead consistent with an energy over temperature, E/T, scaling of the quantum-critical single-electron fluctuation spectrum. Our results provide evidence that the quantum-dynamical scaling and a critical Kondo breakdown simultaneously operate in the same material. Correspondingly, we infer that macroscopic scale-invariant fluctuations emerge from the microscopic many-body excitations associated with a collapsing Fermi-surface. This insight is expected to be relevant to the unconventional finite-temperature behavior in a broad range of strongly correlated quantum systems.


Assuntos
Metais/química , Modelos Químicos , Transição de Fase , Algoritmos , Fenômenos Químicos , Cinética , Magnetismo , Rubídio/química , Dióxido de Silício/química , Temperatura de Transição , Itérbio/química
10.
Chemphyschem ; 11(12): 2639-44, 2010 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-20632351

RESUMO

Single crystals of HfAs(1.7)Se(0.2) are grown by chemical transport reaction and their chemical composition characterized in detail by various analytical methods. Chemical analyses and crystal structure investigations by single-crystal X-ray diffraction as well as powder diffraction with synchrotron radiation reveal a tetragonal PbFCl structure type with strong disorder caused by a significant arsenic deficiency (As(0.9)) on the 2a site and mixed occupancy of the 2c site (As(0.8)Se(0.2)). HfAs(1.7)Se(0.2) is a diamagnetic metal which transforms into a superconducting state at T(c)=0.52 K. Similar to other PbFCl-type arsenide selenides, the title compound displays a magnetic-field-independent -AT(1/2) term in the low-temperature electrical resistivity. This unusual term presumably originates from the electron scattering of structural two-level systems. According to the experimental results, HfAs1.7Se0.2 appears to be a rare example of a nonmagnetic Kondo material.

11.
ACS Nano ; 4(7): 4283-91, 2010 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-20575504

RESUMO

We report a solution-processed, ligand-supported synthesis of 15-20 nm thick Sb(2-x)BixTe3 nanoplatelets. After complete ligand removal by a facile NH3-based etching procedure, the platelets are spark plasma sintered to a p-type nanostructured bulk material with preserved crystal grain sizes. Due to this nanostructure, the total thermal conductivity is reduced by 60% in combination with a reduction in electric conductivity of as low as 20% as compared to the bulk material demonstrating the feasibility of the phonon-glass electron-crystal concept. An enhancement in the dimensionless thermoelectric figure of merit of up to 15% over state-of-the-art bulk materials is achieved, meanwhile, shifting the maximum to significantly higher temperatures.

12.
Phys Rev Lett ; 104(9): 096401, 2010 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-20366998

RESUMO

We present low-temperature thermopower results, S(T), on the heavy-fermion compound YbRh2Si2 in the vicinity of its field-induced quantum critical point (QCP). At B=0, a logarithmic increase of -S(T)/T between 1 and 0.1 K reveals strong non-Fermi-liquid behavior. A pronounced downturn of -S(T)/T below T{max}=0.1 K and a sign change from negative to positive S(T) values at T{0} approximately 30 mK are observed on the low-field side of the Kondo breakdown crossover line T{*}(B). In the field-induced, heavy Landau-Fermi-liquid regime, S(T)/T assumes constant, negative values below T{LFL}. A pronounced crossover in the -S(B)/T isotherms at T{*}(B) sharpens with decreasing T and seems to evolve toward a steplike function for T-->0. This is attributed to an abrupt change of the Fermi volume upon crossing the unconventional QCP of YbRh2Si2.

13.
Dalton Trans ; 39(4): 1012-9, 2010 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-20066185

RESUMO

FeSb(2) was recently identified as a narrow-gap semiconductor with indications of strong electron-electron correlations. In this manuscript, we report on systematic thermoelectric investigation of a number of FeSb(2) single crystals with varying carrier concentrations, together with two isoelectronically substituted FeSb(2-x)As(x) samples (x = 0.01 and 0.03) and two reference compounds FeAs(2) and RuSb(2). Typical behaviour associated with narrow bands and narrow gaps is only confirmed for the FeSb(2) and the FeSb(2-x)As(x) samples. The maximum absolute thermopower of FeSb(2) spans from 10 to 45 mV/K at around 10 K, greatly exceeding that of both FeAs(2) and RuSb(2). The relation between the carrier concentration and the maximum thermopower value is in approximate agreement with theoretical predictions of the electron-diffusion contribution which, however, requires an enhancement factor larger than 30. The isoelectronic substitution leads to a reduction of the thermal conductivity, but the charge-carrier mobility is also largely reduced due to doping-induced crystallographic defects or impurities. In combination with the high charge-carrier mobility and the enhanced thermoelectricity, FeSb(2) represents a promising candidate for thermoelectric cooling applications at cryogenic temperatures.

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