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Register a new userUnusual size effects on thermoelectricity in a strongly correlated oxide
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Added by
Jayakanth Ravichandran
Publication date
2012
fields
Physics
and research's language is
English
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We investigated size effects on thermoelectricity in thin films of a strongly correlated layered cobaltate. At room temperature, the thermopower is independent of thickness down to 6 nm. This unusual behavior is inconsistent with the Fuchs-Sondheimer theory, which is used to describe conventional metals and semiconductors, and is attributed to the strong electron correlations in this material. Although the resistivity increases, as expected, below a critical thickness of $sim$ 30 nm. The temperature dependent thermopower is similar for different thicknesses but resistivity shows systematic changes with thickness. Our experiments highlight the differences in thermoelectric behavior of strongly correlated and uncorrelated systems when subjected to finite size effects. We use the atomic limit Hubbard model at the high temperature limit to explain our observations. These findings provide new insights on decoupling electrical conductivity and thermopower in correlated systems.
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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.
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.
We calculate ground-state energies and density distributions of Hubbard superlattices characterized by periodic modulations of the on-site interaction and the on-site potential. Both density-matrix renormalization group and density-functional methods are employed and compared. We find that small variations in the on-site potential $v_i$ can simulate, cancel, or even overcompensate effects due to much larger variations in the on-site interaction $U_i$. Our findings highlight the importance of nanoscale spatial inhomogeneity in strongly correlated systems, and call for reexamination of model calculations assuming spatial homogeneity.
We report on susceptibility measurements in the strongly correlated layered cobalt oxide [BiBa0.66K0.36O2]CoO2, which demonstrate the existence of a magnetic quantum critical point (QCP) governing the electronic properties. The investigated low frequency susceptibility displays a scaling behavior with both the temperature T and the magnetic field B ranging from the high-T non-Fermi liquid down to the low-T Fermi liquid. Whereas the inferred scaling form can be discussed within the standard framework of the quantum critical phenomena, the determined critical exponents suggest an unconventional magnetic QCP of a potentially generic type. Accordingly, these quantum critical fluctuations account for the anomalous logarithmic temperature dependence of the thermopower. This result allows us to conjecture that quantum criticality can be an efficient source of enhanced thermopower.
We report infrared spectroscopic properties of the strongly correlated layered cobalt oxide [BiBa$_{0.66}$K$_{0.36}$O$_2$]CoO$_2$. These measurements performed on single crystals allow us to determine the optical conductivity as a function of temperature. In addition to a large temperature dependent transfer of spectral weight, an unconventional low energy mode is found. We show that both its frequency and damping scale as the temperature itself. In fact, a basic analysis demonstrates that this mode fully scales onto a function of $omega$/T up to room temperature. This behavior suggests low energy excitations of non-Fermi liquid type originating from quantum criticality.
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