author_facet Yazdani, Sajad
Huan, Tran Doan
Liu, Yufei
Kashfi-Sadabad, Raana
Montaño, Raul David
He, Jian
Pettes, Michael Thompson
Yazdani, Sajad
Huan, Tran Doan
Liu, Yufei
Kashfi-Sadabad, Raana
Montaño, Raul David
He, Jian
Pettes, Michael Thompson
author Yazdani, Sajad
Huan, Tran Doan
Liu, Yufei
Kashfi-Sadabad, Raana
Montaño, Raul David
He, Jian
Pettes, Michael Thompson
spellingShingle Yazdani, Sajad
Huan, Tran Doan
Liu, Yufei
Kashfi-Sadabad, Raana
Montaño, Raul David
He, Jian
Pettes, Michael Thompson
APL Materials
Highly charged interface trap states in PbS1−x govern electro-thermal transport
General Engineering
General Materials Science
author_sort yazdani, sajad
spelling Yazdani, Sajad Huan, Tran Doan Liu, Yufei Kashfi-Sadabad, Raana Montaño, Raul David He, Jian Pettes, Michael Thompson 2166-532X AIP Publishing General Engineering General Materials Science http://dx.doi.org/10.1063/1.5096786 <jats:p>This work describes our discovery of the dominant role of highly charged interfaces on the electrothermal transport properties of PbS, along with a method to reduce the barrier potential for charge carriers by an order of magnitude. High temperature thermoelectrics such as PbS are inevitably exposed to elevated temperatures during postsynthesis treatment as well as operation. However, we observed that as the material was heated, large concentrations of sulfur vacancy (VS̈) sites were formed at temperatures as low as 266 °C. This loss of sulfur doped the PbS n-type and increased the carrier concentration, where these excess electrons were trapped and immobilized at interfacial defect sites in polycrystalline PbS with an abundance of grain boundaries. Sulfur deficient PbS0.81 exhibited a large barrier potential for charge carriers of 0.352 eV, whereas annealing the material under a sulfur-rich environment prevented VS̈ formation and lowered the barrier by an order of magnitude to 0.046 eV. Through ab initio calculations, the formation of VS̈ was found to be more favorable on the surface compared to the bulk of the material with a 1.72 times lower formation energy barrier. These observations underline the importance of controlling interface-vacancy effects in the preparation of bulk materials comprised of nanoscale constituents.</jats:p> Highly charged interface trap states in PbS1−<i>x</i> govern electro-thermal transport APL Materials
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title Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_unstemmed Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_full Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_fullStr Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_full_unstemmed Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_short Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_sort highly charged interface trap states in pbs1−<i>x</i> govern electro-thermal transport
topic General Engineering
General Materials Science
url http://dx.doi.org/10.1063/1.5096786
publishDate 2019
physical
description <jats:p>This work describes our discovery of the dominant role of highly charged interfaces on the electrothermal transport properties of PbS, along with a method to reduce the barrier potential for charge carriers by an order of magnitude. High temperature thermoelectrics such as PbS are inevitably exposed to elevated temperatures during postsynthesis treatment as well as operation. However, we observed that as the material was heated, large concentrations of sulfur vacancy (VS̈) sites were formed at temperatures as low as 266 °C. This loss of sulfur doped the PbS n-type and increased the carrier concentration, where these excess electrons were trapped and immobilized at interfacial defect sites in polycrystalline PbS with an abundance of grain boundaries. Sulfur deficient PbS0.81 exhibited a large barrier potential for charge carriers of 0.352 eV, whereas annealing the material under a sulfur-rich environment prevented VS̈ formation and lowered the barrier by an order of magnitude to 0.046 eV. Through ab initio calculations, the formation of VS̈ was found to be more favorable on the surface compared to the bulk of the material with a 1.72 times lower formation energy barrier. These observations underline the importance of controlling interface-vacancy effects in the preparation of bulk materials comprised of nanoscale constituents.</jats:p>
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author Yazdani, Sajad, Huan, Tran Doan, Liu, Yufei, Kashfi-Sadabad, Raana, Montaño, Raul David, He, Jian, Pettes, Michael Thompson
author_facet Yazdani, Sajad, Huan, Tran Doan, Liu, Yufei, Kashfi-Sadabad, Raana, Montaño, Raul David, He, Jian, Pettes, Michael Thompson, Yazdani, Sajad, Huan, Tran Doan, Liu, Yufei, Kashfi-Sadabad, Raana, Montaño, Raul David, He, Jian, Pettes, Michael Thompson
author_sort yazdani, sajad
container_issue 7
container_start_page 0
container_title APL Materials
container_volume 7
description <jats:p>This work describes our discovery of the dominant role of highly charged interfaces on the electrothermal transport properties of PbS, along with a method to reduce the barrier potential for charge carriers by an order of magnitude. High temperature thermoelectrics such as PbS are inevitably exposed to elevated temperatures during postsynthesis treatment as well as operation. However, we observed that as the material was heated, large concentrations of sulfur vacancy (VS̈) sites were formed at temperatures as low as 266 °C. This loss of sulfur doped the PbS n-type and increased the carrier concentration, where these excess electrons were trapped and immobilized at interfacial defect sites in polycrystalline PbS with an abundance of grain boundaries. Sulfur deficient PbS0.81 exhibited a large barrier potential for charge carriers of 0.352 eV, whereas annealing the material under a sulfur-rich environment prevented VS̈ formation and lowered the barrier by an order of magnitude to 0.046 eV. Through ab initio calculations, the formation of VS̈ was found to be more favorable on the surface compared to the bulk of the material with a 1.72 times lower formation energy barrier. These observations underline the importance of controlling interface-vacancy effects in the preparation of bulk materials comprised of nanoscale constituents.</jats:p>
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spelling Yazdani, Sajad Huan, Tran Doan Liu, Yufei Kashfi-Sadabad, Raana Montaño, Raul David He, Jian Pettes, Michael Thompson 2166-532X AIP Publishing General Engineering General Materials Science http://dx.doi.org/10.1063/1.5096786 <jats:p>This work describes our discovery of the dominant role of highly charged interfaces on the electrothermal transport properties of PbS, along with a method to reduce the barrier potential for charge carriers by an order of magnitude. High temperature thermoelectrics such as PbS are inevitably exposed to elevated temperatures during postsynthesis treatment as well as operation. However, we observed that as the material was heated, large concentrations of sulfur vacancy (VS̈) sites were formed at temperatures as low as 266 °C. This loss of sulfur doped the PbS n-type and increased the carrier concentration, where these excess electrons were trapped and immobilized at interfacial defect sites in polycrystalline PbS with an abundance of grain boundaries. Sulfur deficient PbS0.81 exhibited a large barrier potential for charge carriers of 0.352 eV, whereas annealing the material under a sulfur-rich environment prevented VS̈ formation and lowered the barrier by an order of magnitude to 0.046 eV. Through ab initio calculations, the formation of VS̈ was found to be more favorable on the surface compared to the bulk of the material with a 1.72 times lower formation energy barrier. These observations underline the importance of controlling interface-vacancy effects in the preparation of bulk materials comprised of nanoscale constituents.</jats:p> Highly charged interface trap states in PbS1−<i>x</i> govern electro-thermal transport APL Materials
spellingShingle Yazdani, Sajad, Huan, Tran Doan, Liu, Yufei, Kashfi-Sadabad, Raana, Montaño, Raul David, He, Jian, Pettes, Michael Thompson, APL Materials, Highly charged interface trap states in PbS1−x govern electro-thermal transport, General Engineering, General Materials Science
title Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_full Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_fullStr Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_full_unstemmed Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_short Highly charged interface trap states in PbS1−x govern electro-thermal transport
title_sort highly charged interface trap states in pbs1−<i>x</i> govern electro-thermal transport
title_unstemmed Highly charged interface trap states in PbS1−x govern electro-thermal transport
topic General Engineering, General Materials Science
url http://dx.doi.org/10.1063/1.5096786