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Title: Charge-carrier behavior in Ba-, Sr- and Yb-filled CoSb 3 : NMR and transport studies

Abstract

We report 59Co NMR and transport measurements on n-type filled skutterudites BaxYbyCo4Sb12 and AxCo4Sb12 (A = Ba or Sr), promising thermoelectric materials. The results demonstrate consistently that a shallow defect level near the conduction-band minimum dominates the electronic behavior, in contrast to the behavior of unfilled CoSb3. To analyze the results, we modeled the defect as having a single peak in the density of states, occupied at low temperatures due to donated charges from filler atoms. We fitted the NMR shifts and spin-lattice relaxation rates allowing for arbitrary carrier densities and degeneracies. The results provide a consistent picture for the Hall data, explaining the temperature dependence of the carrier concentration. Furthermore, without adjusting model parameters, we calculated Seebeck coefficient curves, which also provide good consistency. In agreement with recently reported computational results, it appears that composite native defects induced by the presence of filler atoms can explain this behavior. These results provide a better understanding of the balance of charge carriers, which is of crucial importance for designing improved thermoelectric materials.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Solar and Thermal Energy Conversion (CSTEC); Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566689
DOE Contract Number:  
SC0000957
Resource Type:
Journal Article
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 99; Journal Issue: 12; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
solar (photovoltaic), solar (thermal), phonons, thermal conductivity, thermoelectric, electrodes - solar, defects, charge transport, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)

Citation Formats

Tian, Yefan, Sirusi, Ali A., Ballikaya, Sedat, Ghassemi, Nader, Uher, Ctirad, and Ross, Joseph H. Charge-carrier behavior in Ba-, Sr- and Yb-filled CoSb3 : NMR and transport studies. United States: N. p., 2019. Web. doi:10.1103/physrevb.99.125109.
Tian, Yefan, Sirusi, Ali A., Ballikaya, Sedat, Ghassemi, Nader, Uher, Ctirad, & Ross, Joseph H. Charge-carrier behavior in Ba-, Sr- and Yb-filled CoSb3 : NMR and transport studies. United States. doi:10.1103/physrevb.99.125109.
Tian, Yefan, Sirusi, Ali A., Ballikaya, Sedat, Ghassemi, Nader, Uher, Ctirad, and Ross, Joseph H. Fri . "Charge-carrier behavior in Ba-, Sr- and Yb-filled CoSb3 : NMR and transport studies". United States. doi:10.1103/physrevb.99.125109.
@article{osti_1566689,
title = {Charge-carrier behavior in Ba-, Sr- and Yb-filled CoSb3 : NMR and transport studies},
author = {Tian, Yefan and Sirusi, Ali A. and Ballikaya, Sedat and Ghassemi, Nader and Uher, Ctirad and Ross, Joseph H.},
abstractNote = {We report 59Co NMR and transport measurements on n-type filled skutterudites BaxYbyCo4Sb12 and AxCo4Sb12 (A = Ba or Sr), promising thermoelectric materials. The results demonstrate consistently that a shallow defect level near the conduction-band minimum dominates the electronic behavior, in contrast to the behavior of unfilled CoSb3. To analyze the results, we modeled the defect as having a single peak in the density of states, occupied at low temperatures due to donated charges from filler atoms. We fitted the NMR shifts and spin-lattice relaxation rates allowing for arbitrary carrier densities and degeneracies. The results provide a consistent picture for the Hall data, explaining the temperature dependence of the carrier concentration. Furthermore, without adjusting model parameters, we calculated Seebeck coefficient curves, which also provide good consistency. In agreement with recently reported computational results, it appears that composite native defects induced by the presence of filler atoms can explain this behavior. These results provide a better understanding of the balance of charge carriers, which is of crucial importance for designing improved thermoelectric materials.},
doi = {10.1103/physrevb.99.125109},
journal = {Physical Review B},
issn = {2469-9950},
number = 12,
volume = 99,
place = {United States},
year = {2019},
month = {3}
}

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