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Revealing the Intrinsic Electronic Structure of 3D Half-Heusler Thermoelectric Materials by Angle-Resolved Photoemission Spectroscopy

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Fu,  Chenguang
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Yao,  Mengyu
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Li,  Guowei
Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Auffermann,  Gudrun
Gudrun Auffermann, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Burkhardt,  Ulrich
Ulrich Burkhardt, Chemical Metal Science, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Schnelle,  Walter
Walter Schnelle, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Felser,  Claudia
Claudia Felser, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Fu, C., Yao, M., Chen, X., Maulana, L. Z., Li, X., Yang, J., et al. (2019). Revealing the Intrinsic Electronic Structure of 3D Half-Heusler Thermoelectric Materials by Angle-Resolved Photoemission Spectroscopy. Advanced Science, 1902409, pp. 1-8. doi:https://doi.org/10.1002/advs.201902409.


Cite as: http://hdl.handle.net/21.11116/0000-0005-0CB4-3
Abstract
Abstract Accurate determination of the intrinsic electronic structure of thermoelectric materials is a prerequisite for utilizing an electronic band engineering strategy to improve their thermoelectric performance. Herein, with high-resolution angle-resolved photoemission spectroscopy (ARPES), the intrinsic electronic structure of the 3D half-Heusler thermoelectric material ZrNiSn is revealed. An unexpectedly large intrinsic bandgap is directly observed by ARPES and is further confirmed by electrical and optical measurements and first-principles calculations. Moreover, a large anisotropic conduction band with an anisotropic factor of 6 is identified by ARPES and attributed to be one of the most important reasons leading to the high thermoelectric performance of ZrNiSn. These successful findings rely on the grown high-quality single crystals, which have fewer Ni interstitial defects and negligible in-gap states on the electronic structure. This work demonstrates a realistic paradigm to investigate the electronic structure of 3D solid materials by using ARPES and provides new insights into the intrinsic electronic structure of the half-Heusler system benefiting further optimization of thermoelectric performance.