Understanding the complex electronic structure of Mg3Sb2 and the effect of alloying through first-principles tight-binding models
文献信息
Jean-François Halet
Understanding the electronic origin of good thermoelectric (TE) transport properties is a crucial step to design and discover new TE materials. Mg3Sb2 is an intensely researched thermoelectric material, the high TE performance of which comes from six-fold degenerate conduction band minimum at low symmetry k points, leading simultaneously to a high Seebeck coefficient and a good carrier mobility. Furthermore, upon alloying, its low-lying conduction band structure changes, which improves or deteriorates the TE transport properties. Although extensively studied experimentally, the electronic origin of these changes is not well understood. Based on the first-principles derived Wannier function tight-binding analysis of both pristine Mg3Sb2 and its Bi/Ca alloyed derivatives, we reveal that the simple Mg s–Sb p orbital interactions are not adequate and sufficient to describe the electronic structure of Mg3Sb2. Inclusion of both higher energy Mg p orbitals and lower energy Sb s orbitals is demonstrated to be important to understand the shape of the lowest conduction band and its change upon alloying. The systematic chemical understanding developed in this work could enable us to better control the conduction band dispersion by manipulating chemical interactions in Mg3Sb2.
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Journal of Materials Chemistry A

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment










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