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Highly charged interface trap states in PbS1−x govern electro-thermal transport
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Zeitschriftentitel: | APL Materials |
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Personen und Körperschaften: | , , , , , , |
In: | APL Materials, 7, 2019, 7 |
Format: | E-Article |
Sprache: | Englisch |
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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 |
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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 |
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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 |