Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites

Filled skutterudites R x Co 4 Sb 12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-typ...

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Published in:	Nature materials Vol. 14; no. 12; pp. 1223 - 1228
Main Authors:	Tang, Yinglu, Gibbs, Zachary M., Agapito, Luis A., Li, Guodong, Kim, Hyun-Sik, Nardelli, Marco Buongiorno, Curtarolo, Stefano, Snyder, G. Jeffrey
Format:	Journal Article
Language:	English
Published:	London Nature Publishing Group UK 01-12-2015 Nature Publishing Group
Subjects:	119/118 121/135 639/301/1034 639/301/299/2736 Biomaterials Condensed Matter Physics Electronics Heat conductivity High temperature Materials Science Nanotechnology Optical and Electronic Materials solar (photovoltaic), solar (thermal), solid state lighting, phonons, thermal conductivity, thermoelectric, defects, mechanical behavior, charge transport, spin dynamics, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing) Thermal conductivity
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Abstract	Filled skutterudites R x Co 4 Sb 12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb 3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb 3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics. It is shown that the large thermoelectric capability of CoSb 3 skutterudite can be associated with a secondary conduction band with high valley degeneracy, which can converge with the light conduction band at high temperatures.
AbstractList	Filled skutterudites R(x)Co4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics. Filled skutterudites R x Co 4 Sb 12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb 3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb 3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics. It is shown that the large thermoelectric capability of CoSb 3 skutterudite can be associated with a secondary conduction band with high valley degeneracy, which can converge with the light conduction band at high temperatures. Filled skutterudites RxCo4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics.
Author	Tang, Yinglu Curtarolo, Stefano Snyder, G. Jeffrey Gibbs, Zachary M. Kim, Hyun-Sik Li, Guodong Agapito, Luis A. Nardelli, Marco Buongiorno
Author_xml	– sequence: 1 givenname: Yinglu surname: Tang fullname: Tang, Yinglu organization: Department of Materials Science and Engineering, Northwestern University, Materials Science, California Institute of Technology – sequence: 2 givenname: Zachary M. surname: Gibbs fullname: Gibbs, Zachary M. organization: Division of Chemistry and Chemical Engineering, California Institute of Technology – sequence: 3 givenname: Luis A. surname: Agapito fullname: Agapito, Luis A. organization: Department of Physics, University of North Texas, Department of Mechanical Engineering and Materials Science, Physics and Chemistry, Duke University – sequence: 4 givenname: Guodong surname: Li fullname: Li, Guodong organization: Department of Materials Science and Engineering, Northwestern University, Materials Science, California Institute of Technology, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology – sequence: 5 givenname: Hyun-Sik surname: Kim fullname: Kim, Hyun-Sik organization: Department of Materials Science and Engineering, Northwestern University, Materials Science, California Institute of Technology, Materials Research Center, Samsung Advanced Institute of Technology, Samsung Electronics – sequence: 6 givenname: Marco Buongiorno surname: Nardelli fullname: Nardelli, Marco Buongiorno organization: Department of Physics, University of North Texas – sequence: 7 givenname: Stefano surname: Curtarolo fullname: Curtarolo, Stefano organization: Department of Mechanical Engineering and Materials Science, Physics and Chemistry, Duke University – sequence: 8 givenname: G. Jeffrey surname: Snyder fullname: Snyder, G. Jeffrey email: jeff.snyder@northwestern.edu organization: Department of Materials Science and Engineering, Northwestern University, Materials Science, California Institute of Technology
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/26436339$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1370980$$D View this record in Osti.gov
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Snippet	Filled skutterudites R x Co 4 Sb 12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined... Filled skutterudites R(x)Co4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with... Filled skutterudites RxCo4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low...
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StartPage	1223
SubjectTerms	119/118 121/135 639/301/1034 639/301/299/2736 Biomaterials Condensed Matter Physics Electronics Heat conductivity High temperature Materials Science Nanotechnology Optical and Electronic Materials solar (photovoltaic), solar (thermal), solid state lighting, phonons, thermal conductivity, thermoelectric, defects, mechanical behavior, charge transport, spin dynamics, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing) Thermal conductivity
Title	Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb3 skutterudites
URI	https://link.springer.com/article/10.1038/nmat4430 https://www.ncbi.nlm.nih.gov/pubmed/26436339 https://www.proquest.com/docview/1767086332 https://search.proquest.com/docview/1735336081 https://www.osti.gov/biblio/1370980
Volume	14
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