TY - JOUR
T1 - A Chemical Understanding of the Band Convergence in Thermoelectric CoSb3 Skutterudites
T2 - Influence of Electron Population, Local Thermal Expansion, and Bonding Interactions
AU - Hanus, Riley
AU - Guo, Xingyu
AU - Tang, Yinglu
AU - Li, Guodong
AU - Snyder, G. Jeffrey
AU - Zeier, Wolfgang G.
N1 - Funding Information:
G.J.S. and R.H. acknowledge EFRC Solid-State Solar-Thermal Energy Conversion Center (S3TEC) Grant DE-SC0001299. The authors acknowledge the use of the Advanced Photon Source at Argonne National Laboratory for the synchrotron diffraction data, as supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. W.G.Z. acknowledges financial support provided by the DFG via the GrK (Research training group) 2204 “Substitute Materials for sustainable Energy Technologies” as well as the Funds of the Chemical Industry (FCI).
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/2/14
Y1 - 2017/2/14
N2 - N-Type skutterudites, such as YbxCo4Sb12, have recently been shown to exhibit high valley degeneracy with possible band convergence, explaining the excellent thermoelectric efficiency of these materials. Using a combined theoretical and experimental approach involving temperature-dependent synchrotron diffraction, molecular orbital diagrams, and computational studies, the chemical nature of critical features in the band structure is highlighted. We identify how n-type doping on the filler site induces structural changes that are observed in both the diffraction data and computational results. Additionally, we show how chemical n-type doping slightly alters the electronic band structure, moving the high-valley degeneracy secondary conduction band closer to the primary conduction band and thus inducing band convergence.
AB - N-Type skutterudites, such as YbxCo4Sb12, have recently been shown to exhibit high valley degeneracy with possible band convergence, explaining the excellent thermoelectric efficiency of these materials. Using a combined theoretical and experimental approach involving temperature-dependent synchrotron diffraction, molecular orbital diagrams, and computational studies, the chemical nature of critical features in the band structure is highlighted. We identify how n-type doping on the filler site induces structural changes that are observed in both the diffraction data and computational results. Additionally, we show how chemical n-type doping slightly alters the electronic band structure, moving the high-valley degeneracy secondary conduction band closer to the primary conduction band and thus inducing band convergence.
UR - http://www.scopus.com/inward/record.url?scp=85012936605&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85012936605&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.6b04506
DO - 10.1021/acs.chemmater.6b04506
M3 - Article
AN - SCOPUS:85012936605
VL - 29
SP - 1156
EP - 1164
JO - Chemistry of Materials
JF - Chemistry of Materials
SN - 0897-4756
IS - 3
ER -