The reduction of the lattice thermal conductivity is one of the crucial steps in improving thermoelectric materials. In skutterudites, a well-known approach is to reduce the thermal conductivity by filling the structural cage with rare-earth atoms. In this work, we show that it is not just the amount of such filling itself but its nanoscale structuration that lowers the thermal conductivity. A straightforward synthesis procedure under high pressure yields Ce-and Yb-filled CoSb 3 skutterudites, with and without an inhomogeneous distribution of the filler atoms. The composition of the phases is evaluated from synchrotron Xray diffraction (SXRD) data; the highly nanostructured morphology is verified by high-resolution transmission electron microscopy (TEM). The filling fluctuation, i.e., the uneven distribution of filling atoms in the sample originating a phase segregation, brings about low lattice thermal conductivity, as a strong source of phonon scattering. This effect is prominent in the Ce-filled compound, where Ce is segregated into Ce-rich and Ce-poor regions, and the lattice contribution of the thermal conductivity κ L shows a concomitant reduction, approaching values as low as 1.6 W m −1 K −1 at 800 K. Although the level of filling is much higher in Yb x CoSb 3 , its lattice thermal conductivity remains larger. Overall, though, its power factor is enhanced due to charge transfer from the Yb-filler. We thus define a new paradigm for the design of filled skutterudites with exceptionally low thermal conductivities, based on the nanoscale mixing of two phases with different filling factors, spontaneously induced by high-pressure synthesis conditions, which can be considered as pseudoamorphous structures with significant reduction in κ L .
Skutterudite‐type pnictides based on CoSb3 are promising semiconductor materials for thermoelectric applications. An exhaustive structural characterization by synchrotron X‐ray powder diffraction of different M‐filled CoSb3 (M = Y, K, Sr, La, Ce, Yb) skutterudites, with a panoply of M atoms with very different chemical nature, allows to better understand the effects of filling from a crystallo‐chemical point of view. These analyses focus on the correlation of chemical and structural features with the enhanced thermoelectric properties displayed by certain families of filled‐CoSb3 skutterudites. These are mainly determined by Sb positional parameters, yielding Oftedal plots that depend on the filling fraction, ionic state, and atomic radius of the filler. Together with the distortion of [Sb4] rings and [CoSb6] octahedra present in the skutterudite structure, these results are linked to the band‐convergence concept and its influence on the thermoelectric transport properties. Here, the structural changes observed in the different chemical compositions are relevant to understand the improved thermoelectric performance of single partially filled n‐type skutterudites.
Significant control over the properties of a high-carrier density
superconductor via an applied electric field has been considered infeasible
due to screening of the field over atomic length scales. Here, we
demonstrate an enhancement of up to 30% in critical current in a back-gate
tunable NbN micro- and nano superconducting bridges. Our suggested
plausible mechanism of this enhancement in critical current based
on surface nucleation and pinning of Abrikosov vortices is consistent
with expectations and observations for type-II superconductor films
with thicknesses comparable to their coherence length. Furthermore,
we demonstrate an applied electric field-dependent infinite electroresistance
and hysteretic resistance. Our work presents an electric field driven
enhancement in the superconducting property in type-II superconductors
which is a crucial step toward the understanding of field-effects
on the fundamental properties of a superconductor and its exploitation
for logic and memory applications in a superconductor-based low-dissipation
digital computing paradigm.
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