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Register a new userThermopower enhancement by encapsulating cerium in clathrate cages
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Added by
Silke Buehler-Paschen
Publication date
2014
fields
Physics
and research's language is
English
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The increasing worldwide energy consumption calls for the design of more efficient energy systems. Thermoelectrics could be used to convert waste heat back to useful electric energy if only more efficient materials were available. The ideal thermoelectric material combines high electrical conductivity and thermopower with low thermal conductivity. In this regard, the intermetallic type-I clathrates show promise with their exceedingly low lattice thermal conductivities [1]. Here we report the successful incorporation of cerium as guest atom into the clathrate crystal structure. In many simpler intermetallic compounds, this rare earth element is known to lead, via the Kondo interaction, to strong correlation phenomena including the ocurrence of giant thermopowers at low temperatures [2]. Indeed, we observe a 50% enhancement of the thermopower compared to a rare earth-free reference material. Importantly, this enhancement occurs at high temperatures and we suggest that a `rattling enhanced Kondo interaction [3] underlies this effect.
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We have investigated two-dimensional thermoelectric properties in transition metal oxide heterostructures. In particular, we adopted an unprecedented approach to direct tuning of the 2D carrier density using fractionally {delta}-doped oxide superlattices. By artificially controlling the carrier density in the 2D electron gas that emerges at a LaxSr1-xTiO3 {delta}-doped layer, we demonstrate that a thermopower as large as 408 {mu}V K-1 can be reached. This approach also yielded a power factor of the 2D carriers 117 {mu}Wcm-1K-2, which is one of the largest reported values from transition metal oxide based materials. The promising result can be attributed to the anisotropic band structure in the 2D system, indicating that {delta}-doped oxide superlattices can be a good candidate for advanced thermoelectrics.
Lanthanum hydride LaH$_{10}$ with a sodalitelike clathrate structure was experimentally realized to exhibit a room-temperature superconductivity under megabar pressures. Based on first-principles calculations, we reveal that the metal framework of La atoms has the excess electrons at interstitial regions. Such anionic electrons are easily captured to form a stable clathrate structure of H cages. We thus propose that the charge transfer from La to H atoms is mostly driven by the electride property of the La framework. Further, the interaction between La atoms and H cages induces a delocalization of La-5$p$ semicore states to hybridize with H-1$s$ state. Consequently, the bonding nature between La atoms and H cages is characterized as a mixture of ionic and covalent. Our findings demonstrate that anionic and semicore electrons play important roles in stabilizing clathrate H cages in LaH$_{10}$, which can be broadly applicable to other high-pressure rare-earth hydrides with clathrate structures.
We investigate the transport properties of LixCoO2 thin films whose resistivities are nearly an order of magnitude lower than those of the bulk polycrystals. A metal-nonmetal transition occurs at ~0.8 in a biphasic domain, and the Seebeck coefficient (S) is drastically increased at ~140 K (= T*) with increasing the Li concentration to show a peak of magnitude ~120 muV/K in the S-T curve of x = 0.87. We show that T* corresponds to a crossover temperature in the conduction, most likely reflecting the correlation-induced temperature dependence in the low-energy excitations.
High-temperature thermopower is interpreted as entropy that a carrier carries. Owing to spin and orbital degrees of freedom, a transition metal perovskite exhibits large thermopower at high temperatures. In this paper, we revisit the high-temperature thermopower in the perovskites to shed light on the degrees of freedom. Thus, we theoretically derive an expression of thermopower in one-dimensional octahedral-MX6-clusters chain using linear-response theory and electronic structure calculation of the chain based on the tight-binding approximation. The derived expression of the thermopower is consistent with the extended Heikes formula and well reproduced experimental data of several perovskite oxides at high temperatures. In this expression, a degeneracy of many electron states in octahedral ligand field (which is characterized by multiplet term) appears instead of the spin and orbital degeneracies. Complementarity in between our expression and the extended Heikes formula is discussed.
We report giant thermopower S = 2.5 mV/K in CoSbS single crystals, a material that shows strong high-temperature thermoelectric performance when doped with Ni or Se. Changes of low temperature thermopower induced by magnetic field point to mechanism of electronic diffusion of carriers in the heavy valence band. Intrinsic magnetic susceptibility is consistent with the Kondo- Insulator-like accumulation of electronic states around the gap edges. This suggests that giant thermopower stems from temperature-dependent renormalization of the non-interacting bands and buildup of the electronic correlations on cooling.
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