Electronic band structure and low-temperature transport properties of the type-I clathrate Ba<sub>8</sub>Ni<sub>x</sub>Ge<sub>46-x-y</sub>□<sub>y</sub> - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Dalton Transactions Année : 2015

Electronic band structure and low-temperature transport properties of the type-I clathrate Ba8NixGe46-x-yy

Résumé

We present the evolution of the low-temperature thermodynamic, galvanomagnetic and thermoelectric properties of the type-I clathrate Ba8NixGe46-x-yy with the Ni concentration studied on polycrystalline samples with 0.0 <= x <= 6.0 by means of specific heat, Hall effect, electrical resistivity, thermopower and thermal conductivity measurements in the 2-350 K temperature range and supported by first-principles calculations. The experimental results evidence a 2a x 2a x 2a supercell described in the space group Ia-3d for x <= 1.0 and a primitive unit cell a x a x a (space group Pm-3n) above this Ni content. This concentration also marks the limit between a regime where both electrons and holes contribute to the electrical conduction (x <= 1.0) and a conventional, single-carrier regime (x > 1.0). This evolution is traced by the variations in the thermopower and Hall effect with x. In agreement with band structure calculations, increasing the Ni content drives the system from a nearly-compensated semimetallic state (x = 0.0) towards a narrow-band-gap semiconducting state (x = 4.0). A crossover from an n-type to a p-type conduction occurs when crossing the x = 4.0 concentration i.e. for x = 4.1. The solid solution Ba8NixGe46-x-yy therefore provides an excellent experimental platform to probe the evolution of the peculiar properties of the parent type-I clathrate Ba8Ge433 upon Ge/Ni substitution and filling up of the vacancies, which might be universal among the ternary systems at low substitution levels.
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hal-01280798 , version 1 (20-02-2023)

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Umut Aydemir, Christophe Candolfi, Alim Ormeci, Michael Baitinger, Ulrich Burkhardt, et al.. Electronic band structure and low-temperature transport properties of the type-I clathrate Ba8NixGe46-x-yy. Dalton Transactions, 2015, 44 (16), pp.7524-7537. ⟨10.1039/c4dt03827d⟩. ⟨hal-01280798⟩
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