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Register a new userThermoelectricity in correlated narrow-gap semiconductors
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Authors
Jan M. Tomczak
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We review many-body effects, their microscopic origin, as well as their impact onto thermoelectricity in correlated narrow-gap semiconductors. Members of this class---such as FeSi and FeSb$_2$---display an unusual temperature dependence in various observables: insulating with large thermopowers at low temperatures, they turn bad metals at temperatures much smaller than the size of their gaps. This insulator-to-metal crossover is accompanied by spectral weight-transfers over large energies in the optical conductivity and by a gradual transition from activated to Curie-Weiss-like behaviour in the magnetic susceptibility. We show a retrospective of the understanding of these phenomena, discuss the relation to heavy-fermion Kondo insulators---such as Ce$_3$Bi$_4$Pt$_3$ for which we present new results---and propose a general classification of paramagnetic insulators. From the latter FeSi emerges as an orbital-selective Kondo insulator. Focussing on intermetallics such as silicides, antimonides, skutterudites, and Heusler compounds we showcase successes and challenges for the realistic simulation of transport properties in the presence of electronic correlations. Further, we advert to new avenues in which electronic correlations may contribute to the improvement of thermoelectric performance.
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Iron based narrow gap semiconductors such as FeSi, FeSb2, or FeGa3 have received a lot of attention because they exhibit a large thermopower, as well as striking similarities to heavy fermion Kondo insulators. Many proposals have been advanced, however, lacking quantitative methodologies applied to this problem, a consensus remained elusive to date. Here, we employ realistic many-body calculations to elucidate the impact of electronic correlation effects on FeSi. Our methodology accounts for all substantial anomalies observed in FeSi: the metallization, the lack of conservation of spectral weight in optical spectroscopy, and the Curie susceptibility. In particular we find a very good agreement for the anomalous thermoelectric power. Validated by this congruence with experiment, we further discuss a new physical picture of the microscopic nature of the insulator-to-metal crossover. Indeed, we find the suppression of the Seebeck coefficient to be driven by correlation induced incoherence. Finally, we compare FeSi to its iso-structural and iso-electronic homologue RuSi, and predict that partially substituted Fe(1-x)Ru(x)Si will exhibit an increased thermopower at intermediate temperatures.
The search for semiconductors with high thermoelectric figure of merit has been greatly aided by theoretical modeling of electron and phonon transport, both in bulk materials and in nanocomposites. Recent experiments have studied thermoelectric transport in ``strongly correlated materials derived by doping Mott insulators, whose insulating behavior without doping results from electron-electron repulsion, rather than from band structure as in semiconductors. Here a unified theory of electrical and thermal transport in the atomic and ``Heikes limit is applied to understand recent transport experiments on sodium cobaltate and other doped Mott insulators at room temperature and above. For optimal electron filling, a broad class of narrow-bandwidth correlated materials are shown to have power factors (the electronic portion of the thermoelectric figure of merit) as high at and above room temperature as in the best semiconductors.
Highly unconventional behavior of the thermodynamic response functions has been experimentally observed in a narrow gap semiconductor samarium hexaboride. Motivated by these observations, we use renormalization group technique to investigate many-body instabilities in the f-orbital narrow gap semiconductors with band inversion in the limit of weak coupling. After projecting out the double occupancy of the f-orbital states, we formulate a low-energy theory describing the interacting particles in two hybridized electron- and hole-like bands. The interactions are assumed to be weak and short-ranged. We take into account the difference between the effective masses of the quasiparticles in each band. Upon carrying out the renormalization group analysis we find that there is only one stable fixed point corresponding to the excitonic instability with time-reversal symmetry breaking for small enough mismatch between the effective masses.
A study of the anisotropy in magnetic, transport and magnetotransport properties of FeSb2 has been made on large single crystals grown from Sb flux. Magnetic susceptibility of FeSb2 shows diamagnetic to paramagnetic crossover around 100K. Electrical transport along two axes is semiconducting whereas the third axis exhibits a metal - semiconductor crossover at temperature Tmin which is sensitive to current alignment and ranges between 40 and 80K. In H=70kOe semiconducting transport is restored for T<300K, resulting in large magnetoresistance [rho(70kOe)-rho(0)]/rho(0)=2200% in the crossover temperature range
We report inelastic neutron scattering measurements aimed at investigating the origin of the temperature-induced paramagnetism in the narrow-gap semiconductor FeSb2. We find that inelastic response for energies up to 60 meV and at temperatures 4.2 K, 300 K and 550 K is essentially consistent with the scattering by lattice phonon excitations. We observe no evidence for a well-defined magnetic peak corresponding to the excitation from the non-magnetic S = 0 singlet ground state to a state of magnetic multiplet in the localized spin picture. Our data establish the quantitative limit of S_{eff}^2 < 0.25 on the fluctuating local spin. However, a broad magnetic scattering continuum in the 15 meV to 35 meV energy range is not ruled out by our data. Our findings make description in terms of the localized Fe spins unlikely and suggest that paramagnetic susceptibility of itinerant electrons is at the origin of the temperature-induced magnetism in FeSb2.
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