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Journal Article

Engineering Transport Properties in Interconnected Enargite-Stannite Type Cu2+xMn1−xGeS4 Nanocomposites


Le Tonquesse,  S.
Chemical Metal Science, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Pavan Kumar, V., Passuti, S., Zhang, B., Fujii, S., Yoshizawa, K., Boullay, P., et al. (2022). Engineering Transport Properties in Interconnected Enargite-Stannite Type Cu2+xMn1−xGeS4 Nanocomposites. Angewandte Chemie, International Edition in English, 61(49): e202210600, pp. 1-12. doi:10.1002/anie.202210600.

Cite as: https://hdl.handle.net/21.11116/0000-000C-3915-D
Understanding the mechanisms that connect heat and electron transport with crystal structures and defect chemistry is fundamental to develop materials with thermoelectric properties. In this work, we synthesized a series of self-doped compounds Cu2+xMn1−xGeS4 through Cu for Mn substitution. Using a combination of powder X-ray diffraction, high resolution transmission electron microscopy and precession-assisted electron diffraction tomography, we evidence that the materials are composed of interconnected enargite- and stannite-type structures, via the formation of nanodomains with a high density of coherent interfaces. By combining experiments with ab initio electron and phonon calculations, we discuss the structure–thermoelectric properties relationships and clarify the interesting crystal chemistry in this system. We demonstrate that excess Cu+ substituted for Mn2+ dopes holes into the top of the valence band, leading to a remarkable enhancement of the power factor and figure of merit ZT. © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.