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Title: Solubility limits in quaternary SnTe-based alloys [Metastability and solubility limits in quaternary SnTe-based alloys guided by combinatorial sputtering]

Abstract

Here, the controlled decomposition of metastable alloys is an attractive route to form nanostructured thermoelectric materials with reduced thermal conductivity. The ternary SnTe–MnTe and SnTe–SnSe heterostructural alloys have been demonstrated as promising materials for thermoelectric applications. In this work, the quaternary Sn1–yMnyTe1–xSex phase space serves as a relevant model system to explore how a combination of computational and combinatorial-growth methods can be used to study equilibrium and non-equilibrium solubility limits. Results from first principle calculations indicate low equilibrium solubility for x,y < 0.05 that are in good agreement with results obtained from bulk equilibrium synthesis experiments and predict significantly higher spinodal limits. An experimental screening using sputtered combinatorial thin film sample libraries showed a remarkable increase in non-equilibrium solubility for x,y > 0.2. These theoretical and experimental results were used to guide the bulk synthesis of metastable alloys. The ability to reproduce the non-equilibrium solubility levels in bulk materials indicates that such theoretical calculations and combinatorial growth can inform bulk synthetic routes. Further, the large difference between equilibrium and non-equilibrium solubility limits in Sn1–yMnyTe1–xSex indicates these metastable alloys are attractive in terms of nano-precipitate formation for potential thermoelectric applications.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  3. Colorado School of Mines, Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), NREL Laboratory Directed Research and Development (LDRD); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1360667
Report Number(s):
NREL/JA-5K00-68341
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 7; Journal Issue: 40; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; thermoelectric materials; thermal conductivity; decomposition; alloys; SnTe; MnSe; MnTe; SnSe; non equilibrium; solubility; combinatorial sputtering; high throughput; computational phase diagram; quaternary alloys

Citation Formats

Siol, Sebastian, Holder, Aaron, Ortiz, Brenden R., Parilla, Philip A., Toberer, Eric, Lany, Stephan, and Zakutayev, Andriy. Solubility limits in quaternary SnTe-based alloys [Metastability and solubility limits in quaternary SnTe-based alloys guided by combinatorial sputtering]. United States: N. p., 2017. Web. doi:10.1039/C6RA28219A.
Siol, Sebastian, Holder, Aaron, Ortiz, Brenden R., Parilla, Philip A., Toberer, Eric, Lany, Stephan, & Zakutayev, Andriy. Solubility limits in quaternary SnTe-based alloys [Metastability and solubility limits in quaternary SnTe-based alloys guided by combinatorial sputtering]. United States. doi:10.1039/C6RA28219A.
Siol, Sebastian, Holder, Aaron, Ortiz, Brenden R., Parilla, Philip A., Toberer, Eric, Lany, Stephan, and Zakutayev, Andriy. Tue . "Solubility limits in quaternary SnTe-based alloys [Metastability and solubility limits in quaternary SnTe-based alloys guided by combinatorial sputtering]". United States. doi:10.1039/C6RA28219A. https://www.osti.gov/servlets/purl/1360667.
@article{osti_1360667,
title = {Solubility limits in quaternary SnTe-based alloys [Metastability and solubility limits in quaternary SnTe-based alloys guided by combinatorial sputtering]},
author = {Siol, Sebastian and Holder, Aaron and Ortiz, Brenden R. and Parilla, Philip A. and Toberer, Eric and Lany, Stephan and Zakutayev, Andriy},
abstractNote = {Here, the controlled decomposition of metastable alloys is an attractive route to form nanostructured thermoelectric materials with reduced thermal conductivity. The ternary SnTe–MnTe and SnTe–SnSe heterostructural alloys have been demonstrated as promising materials for thermoelectric applications. In this work, the quaternary Sn1–yMnyTe1–xSex phase space serves as a relevant model system to explore how a combination of computational and combinatorial-growth methods can be used to study equilibrium and non-equilibrium solubility limits. Results from first principle calculations indicate low equilibrium solubility for x,y < 0.05 that are in good agreement with results obtained from bulk equilibrium synthesis experiments and predict significantly higher spinodal limits. An experimental screening using sputtered combinatorial thin film sample libraries showed a remarkable increase in non-equilibrium solubility for x,y > 0.2. These theoretical and experimental results were used to guide the bulk synthesis of metastable alloys. The ability to reproduce the non-equilibrium solubility levels in bulk materials indicates that such theoretical calculations and combinatorial growth can inform bulk synthetic routes. Further, the large difference between equilibrium and non-equilibrium solubility limits in Sn1–yMnyTe1–xSex indicates these metastable alloys are attractive in terms of nano-precipitate formation for potential thermoelectric applications.},
doi = {10.1039/C6RA28219A},
journal = {RSC Advances},
number = 40,
volume = 7,
place = {United States},
year = {2017},
month = {5}
}

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