Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics

Abstract Coinage metals Cu and Ag are widely reckoned as effective dopants in thermoelectric materials due to their ability to optimise carrier concentration while preserving high carrier mobility, attributed to their inherent dynamic features. Traditionally, Cu/Ag ions are introduced through eutect...

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Main Authors: Yongqi Chen, Meng Li, Xiaodong Wang, Wenyi Chen, Siqi Liu, Min Zhang, Wanyu Lyu, Nanhai Li, Han Gao, Weidi Liu, Xiao-Lei Shi, Zhi-Gang Chen
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-62078-1
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author Yongqi Chen
Meng Li
Xiaodong Wang
Wenyi Chen
Siqi Liu
Min Zhang
Wanyu Lyu
Nanhai Li
Han Gao
Weidi Liu
Xiao-Lei Shi
Zhi-Gang Chen
author_facet Yongqi Chen
Meng Li
Xiaodong Wang
Wenyi Chen
Siqi Liu
Min Zhang
Wanyu Lyu
Nanhai Li
Han Gao
Weidi Liu
Xiao-Lei Shi
Zhi-Gang Chen
author_sort Yongqi Chen
collection DOAJ
description Abstract Coinage metals Cu and Ag are widely reckoned as effective dopants in thermoelectric materials due to their ability to optimise carrier concentration while preserving high carrier mobility, attributed to their inherent dynamic features. Traditionally, Cu/Ag ions are introduced through eutectic reactions, which inevitably result in interstitial doping. Here, we develop an innovative solid solution doping strategy that enables targeted doping, whereby Cu ions exclusively occupy host lattice sites rather than interstitial sites. By combining first-principles calculations with in-situ experiments, we demonstrate that this targeted doping approach relies on ion diffusion and induces lattice renormalisation, effectively reducing lattice defects and suppressing hole concentration. Consequently, the 1 at.% Cu doped Ge0.85Sb0.10Te sample exhibits an exceptional figure-of-merit of 2.3 at 775 K along with a desirable average value of 1.4 scoping 300 to 775 K. The power density of the corresponding single-leg thermoelectric module is 2.23 W·cm−2 under a temperature difference of 475 K. This work not only explains the kinetics behind dynamic doping behaviours, but also provide an original method to achieve high-quality functional materials with less lattice defects and a high carrier mobility.
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spelling doaj-art-eb20fb0d39504e0d96d5c3dd8d4d1ddc2025-08-20T04:02:55ZengNature PortfolioNature Communications2041-17232025-07-0116111010.1038/s41467-025-62078-1Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectricsYongqi Chen0Meng Li1Xiaodong Wang2Wenyi Chen3Siqi Liu4Min Zhang5Wanyu Lyu6Nanhai Li7Han Gao8Weidi Liu9Xiao-Lei Shi10Zhi-Gang Chen11School of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologyCentral Analytical Research Facility, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologySchool of Chemistry and Physics, ARC Research Hub in Zero-emission Power Generation for Carbon Neutrality, and Centre for Materials Science, Queensland University of TechnologyAbstract Coinage metals Cu and Ag are widely reckoned as effective dopants in thermoelectric materials due to their ability to optimise carrier concentration while preserving high carrier mobility, attributed to their inherent dynamic features. Traditionally, Cu/Ag ions are introduced through eutectic reactions, which inevitably result in interstitial doping. Here, we develop an innovative solid solution doping strategy that enables targeted doping, whereby Cu ions exclusively occupy host lattice sites rather than interstitial sites. By combining first-principles calculations with in-situ experiments, we demonstrate that this targeted doping approach relies on ion diffusion and induces lattice renormalisation, effectively reducing lattice defects and suppressing hole concentration. Consequently, the 1 at.% Cu doped Ge0.85Sb0.10Te sample exhibits an exceptional figure-of-merit of 2.3 at 775 K along with a desirable average value of 1.4 scoping 300 to 775 K. The power density of the corresponding single-leg thermoelectric module is 2.23 W·cm−2 under a temperature difference of 475 K. This work not only explains the kinetics behind dynamic doping behaviours, but also provide an original method to achieve high-quality functional materials with less lattice defects and a high carrier mobility.https://doi.org/10.1038/s41467-025-62078-1
spellingShingle Yongqi Chen
Meng Li
Xiaodong Wang
Wenyi Chen
Siqi Liu
Min Zhang
Wanyu Lyu
Nanhai Li
Han Gao
Weidi Liu
Xiao-Lei Shi
Zhi-Gang Chen
Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
Nature Communications
title Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
title_full Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
title_fullStr Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
title_full_unstemmed Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
title_short Copper ion diffusion by solid solution treatment advancing GeTe-based thermoelectrics
title_sort copper ion diffusion by solid solution treatment advancing gete based thermoelectrics
url https://doi.org/10.1038/s41467-025-62078-1
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