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Correlated evolution of colossal thermoelectric effect and Kondo insulating behavior
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Figures

Image of FIG. 1.

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FIG. 1.

Evolution of the thermoelectric properties of Fe-doped RuSb. (a) Seebeck coefficient () as a function of temperature and composition. The data for FeSb ( = 1) are towards the front, while RuSb ( = 0) has been projected onto the back wall. With more Fe, the peak shifts to lower and becomes larger and narrower. (b) Value of the Seebeck coefficient peak as a function of composition. = 0.10 and 0.20 samples are included here but not in the previous panel to preserve the latter's clarity. (c) Thermoelectric power factor ( = 2/) as a function of . The v-shaped features mark crossovers between -type and -type transports (closed and open circles, respectively) at temperatures corresponding to sign changes in . The composition can be tuned to make - or -type thermoelements for different temperature ranges.

Image of FIG. 2.

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FIG. 2.

Evolution of the electrical resistivity () with composition. With more Fe, the resistivity decreases at all temperatures and thus enhances the thermoelectric performance. In each curve containing Fe, the shoulder between the two distinct exponential behaviors is a signature of the Kondo effect. Left inset: In the high- regime, the decrease in slope with Fe content indicates a decrease in the band gap. = 0.10 and 0.20 samples are included here but not in the main panel to preserve the latter's clarity. Right inset: Due to the decreased band gap, greater Fe content also causes the room temperature to decrease exponentially (left axis), while the -type carrier concentration increases exponentially (right axis).

Image of FIG. 3.

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FIG. 3.

In Fe-containing samples, the magnetic susceptibility () transitions from diamagnetism to a thermally enhanced Pauli-like paramagnetism with heating. The = 0 (RuSb) sample is purely diamagnetic and decreases slightly with . In the others, the approximate transition temperature ( ) is indicated by the arrows to occur at the minimum of each curve, which moves to lower as Fe is added. At very low (upper inset) the small Curie tails indicate the sample purity, and the flatter, diamagnetic portions of the curves systematically increase, linearly depending on the Fe content (lower left inset). At 300 K, the paramagnetic signal also linearly increases with more Fe.

Image of FIG. 4.

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FIG. 4.

Electronic structure calculations. Fe doping enhances the density of -states near , causing both the conduction and valence bands to become more localized. Left inset: Band structure of the theoretical compound with = 0.0625, where heavy plotting represents -states that are solely due to Fe. The flat portions of the curves illustrate the partially localized character of these states. Right inset: The experimental lattice parameters for comparison to the corresponding electronic structures and to indicate the unit cell dimensions for the calculations.

Image of FIG. 5.

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FIG. 5.

Selected transition temperatures from all the properties. At low , all samples exhibit behavior type I, where they are all diamagnetic, have a negative that increases in magnitude with , and follow the small activation gap in their electronic conduction. Heating all samples leads eventually to behavior type II via the following progression: a change from diamagnetism to paramagnetism ( , ▽), then a decline in the Seebeck coefficient ( , ●), followed by the transitional shoulder in the resistivity ( , ×), and finally a crossover in the Seebeck coefficient from - to -type ( , □). The errors are about as large as the data points. The thermoelectric properties gradually improve in the direction shown by the arrow, culminating with the colossal Seebeck coefficient peak of FeSb occurring at 12 K (○, Ref. 8 ).

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/content/aip/journal/aplmater/1/6/10.1063/1.4833055
2013-12-02
2014-04-24

Abstract

We report the magnetic and transport properties of the RuFeSb solid solution, showing how the colossal thermoelectric performance of FeSb evolves due to changes in the amount of 3 vs. 4 electron character. The physical property trends shed light on the physical picture underlying one of the best low- thermoelectric power factors known to date. Some of the compositions warrant further study as possible - and -type thermoelements for Peltier cooling well below 300 K. Our findings enable us to suggest possible new Kondo insulating systems that might behave similarly to FeSb as advanced thermoelectrics.

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Scitation: Correlated evolution of colossal thermoelectric effect and Kondo insulating behavior
http://aip.metastore.ingenta.com/content/aip/journal/aplmater/1/6/10.1063/1.4833055
10.1063/1.4833055
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