Defect chemistry and doping of BiCuSeO

Michael Y. Toriyama; Jiaxing Qu; G. Jeffrey Snyder; Prashun Gorai

doi:10.1039/d1ta05112a

Defect chemistry and doping of BiCuSeO

Michael Y. Toriyama^*, Jiaxing Qu, G. Jeffrey Snyder, Prashun Gorai

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

Abstract

While p-type BiCuSeO is a well-known mid-temperature oxide thermoelectric (TE) material, computations predict that superior TE performance can be realized through n-type doping. In this study, we use first-principles defect calculations to show that Cu vacancies are responsible for the native p-type self doping; yet, we find that BiCuSeO is n-type dopable under Cu-rich growth conditions, where the formation of Cu vacancies is suppressed. We computationally survey a broad suite of 23 dopants and find that only Cl and Br are effective n-type dopants. Therefore, we recommend that future experimental doping efforts utilize phase boundary mapping to optimize the electron concentration and resolve the anomalous p-n-p transitions observed in halogen-doped BiCuSeO. The prospect of n-type doping, as revealed by our defect calculations, paves the path for rational design of BiCuSeO chemical analogues with similar doping behavior and even better TE performance.

Original language	English (US)
Pages (from-to)	20685-20694
Number of pages	10
Journal	Journal of Materials Chemistry A
Volume	9
Issue number	36
DOIs	https://doi.org/10.1039/d1ta05112a
State	Published - Sep 28 2021

Funding

MYT is funded by the United States Department of Energy through the Computational Science Graduate Fellowship (DOE CSGF) under grant number DE-SC0020347. JQ is funded by the NSF DIGI-MAT program, grant number 1922758. GJS acknowledges support from NSF DMR, DMREF grant number 1729487 and PG acknowledges support from NSF through award DMR-2102409. The research was performed using computational resources sponsored by the Department of Energy's Office of Energy Efficiency and Renewable Energy and located at the NREL. This research was also supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology.

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1039/d1ta05112a

Cite this

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title = "Defect chemistry and doping of BiCuSeO",

abstract = "While p-type BiCuSeO is a well-known mid-temperature oxide thermoelectric (TE) material, computations predict that superior TE performance can be realized through n-type doping. In this study, we use first-principles defect calculations to show that Cu vacancies are responsible for the native p-type self doping; yet, we find that BiCuSeO is n-type dopable under Cu-rich growth conditions, where the formation of Cu vacancies is suppressed. We computationally survey a broad suite of 23 dopants and find that only Cl and Br are effective n-type dopants. Therefore, we recommend that future experimental doping efforts utilize phase boundary mapping to optimize the electron concentration and resolve the anomalous p-n-p transitions observed in halogen-doped BiCuSeO. The prospect of n-type doping, as revealed by our defect calculations, paves the path for rational design of BiCuSeO chemical analogues with similar doping behavior and even better TE performance.",

author = "Toriyama, {Michael Y.} and Jiaxing Qu and Snyder, {G. Jeffrey} and Prashun Gorai",

note = "Funding Information: MYT is funded by the United States Department of Energy through the Computational Science Graduate Fellowship (DOE CSGF) under grant number DE-SC0020347. JQ is funded by the NSF DIGI-MAT program, grant number 1922758. GJS acknowledges support from NSF DMR, DMREF grant number 1729487 and PG acknowledges support from NSF through award DMR-2102409. The research was performed using computational resources sponsored by the Department of Energy's Office of Energy Efficiency and Renewable Energy and located at the NREL. This research was also supported in part through the computational resources and staff contributions provided for the Quest high performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. Publisher Copyright: {\textcopyright} The Royal Society of Chemistry 2021.",

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AU - Toriyama, Michael Y.

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PY - 2021/9/28

Y1 - 2021/9/28

N2 - While p-type BiCuSeO is a well-known mid-temperature oxide thermoelectric (TE) material, computations predict that superior TE performance can be realized through n-type doping. In this study, we use first-principles defect calculations to show that Cu vacancies are responsible for the native p-type self doping; yet, we find that BiCuSeO is n-type dopable under Cu-rich growth conditions, where the formation of Cu vacancies is suppressed. We computationally survey a broad suite of 23 dopants and find that only Cl and Br are effective n-type dopants. Therefore, we recommend that future experimental doping efforts utilize phase boundary mapping to optimize the electron concentration and resolve the anomalous p-n-p transitions observed in halogen-doped BiCuSeO. The prospect of n-type doping, as revealed by our defect calculations, paves the path for rational design of BiCuSeO chemical analogues with similar doping behavior and even better TE performance.

AB - While p-type BiCuSeO is a well-known mid-temperature oxide thermoelectric (TE) material, computations predict that superior TE performance can be realized through n-type doping. In this study, we use first-principles defect calculations to show that Cu vacancies are responsible for the native p-type self doping; yet, we find that BiCuSeO is n-type dopable under Cu-rich growth conditions, where the formation of Cu vacancies is suppressed. We computationally survey a broad suite of 23 dopants and find that only Cl and Br are effective n-type dopants. Therefore, we recommend that future experimental doping efforts utilize phase boundary mapping to optimize the electron concentration and resolve the anomalous p-n-p transitions observed in halogen-doped BiCuSeO. The prospect of n-type doping, as revealed by our defect calculations, paves the path for rational design of BiCuSeO chemical analogues with similar doping behavior and even better TE performance.

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Defect chemistry and doping of BiCuSeO

Abstract

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