Computational design of thermoelectric alloys through optimization of transport and dopability
Abstract
Alloying is a common technique to optimize the functional properties of materials for thermoelectrics, photovoltaics, energy storage etc. Designing thermoelectric (TE) alloys is especially challenging because it is a multi-property optimization problem, where the properties that contribute to high TE performance are interdependent. In this work, we develop a computational framework that combines first-principles calculations with alloy and point defect modeling to identify alloy compositions that optimize the electronic, thermal, and defect properties. We apply this framework to design n-type Ba2(1–x)Sr2xCdP2 Zintl thermoelectric alloys. Our predictions of the crystallographic properties such as lattice parameters and site disorder are validated with experiments. To optimize the conduction band electronic structure, we perform band unfolding to sketch the effective band structures of alloys and find a range of compositions that facilitate band convergence and minimize alloy scattering of electrons. Here, we assess the n-type dopability of the alloys by extending the standard approach for computing point defect energetics in ordered structures. Through the application of this framework, we identify an optimal alloy composition range with the desired electronic and thermal transport properties, and n-type dopability. Such a computational framework can also be used to design alloys for other functional applications beyond TE.
- Authors:
-
[1];
[2];
[2];
[3]
- University of Illinois at Urbana-Champaign, IL (United States)
- University of Delaware, Newark, DE (United States)
- Colorado School of Mines, Golden, CO (United States)
- Publication Date:
- Research Org.:
- Univ. of Delaware, Newark, DE (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1978806
- Alternate Identifier(s):
- OSTI ID: 1833739
- Grant/Contract Number:
- SC0008885
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Materials Horizons
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 2051-6347
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Chemistry; Materials Science
Citation Formats
Qu, Jiaxing, Balvanz, Adam, Baranets, Sviatoslav, Bobev, Svilen, and Gorai, Prashun. Computational design of thermoelectric alloys through optimization of transport and dopability. United States: N. p., 2021.
Web. doi:10.1039/d1mh01539g.
Qu, Jiaxing, Balvanz, Adam, Baranets, Sviatoslav, Bobev, Svilen, & Gorai, Prashun. Computational design of thermoelectric alloys through optimization of transport and dopability. United States. https://doi.org/10.1039/d1mh01539g
Qu, Jiaxing, Balvanz, Adam, Baranets, Sviatoslav, Bobev, Svilen, and Gorai, Prashun. Fri .
"Computational design of thermoelectric alloys through optimization of transport and dopability". United States. https://doi.org/10.1039/d1mh01539g. https://www.osti.gov/servlets/purl/1978806.
@article{osti_1978806,
title = {Computational design of thermoelectric alloys through optimization of transport and dopability},
author = {Qu, Jiaxing and Balvanz, Adam and Baranets, Sviatoslav and Bobev, Svilen and Gorai, Prashun},
abstractNote = {Alloying is a common technique to optimize the functional properties of materials for thermoelectrics, photovoltaics, energy storage etc. Designing thermoelectric (TE) alloys is especially challenging because it is a multi-property optimization problem, where the properties that contribute to high TE performance are interdependent. In this work, we develop a computational framework that combines first-principles calculations with alloy and point defect modeling to identify alloy compositions that optimize the electronic, thermal, and defect properties. We apply this framework to design n-type Ba2(1–x)Sr2xCdP2 Zintl thermoelectric alloys. Our predictions of the crystallographic properties such as lattice parameters and site disorder are validated with experiments. To optimize the conduction band electronic structure, we perform band unfolding to sketch the effective band structures of alloys and find a range of compositions that facilitate band convergence and minimize alloy scattering of electrons. Here, we assess the n-type dopability of the alloys by extending the standard approach for computing point defect energetics in ordered structures. Through the application of this framework, we identify an optimal alloy composition range with the desired electronic and thermal transport properties, and n-type dopability. Such a computational framework can also be used to design alloys for other functional applications beyond TE.},
doi = {10.1039/d1mh01539g},
journal = {Materials Horizons},
number = 2,
volume = 9,
place = {United States},
year = {Fri Nov 26 00:00:00 EST 2021},
month = {Fri Nov 26 00:00:00 EST 2021}
}
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Works referenced in this record:
U1 snRNP regulates cancer cell migration and invasion in vitro
journal, January 2020
- Oh, Jung-Min; Venters, Christopher C.; Di, Chao
- Nature Communications, Vol. 11, Issue 1
Contrasting SnTe–NaSbTe 2 and SnTe–NaBiTe 2 Thermoelectric Alloys: High Performance Facilitated by Increased Cation Vacancies and Lattice Softening
journal, July 2020
- Slade, Tyler J.; Pal, Koushik; Grovogui, Jann A.
- Journal of the American Chemical Society, Vol. 142, Issue 28
Towards the high-throughput synthesis of bulk materials: thermoelectric PbTe–PbSe–SnTe–SnSe alloys
journal, January 2019
- Ortiz, Brenden R.; Adamczyk, Jesse M.; Gordiz, Kiarash
- Molecular Systems Design & Engineering, Vol. 4, Issue 2
Elasticity and constitution of the Earth's interior
journal, June 1952
- Birch, Francis
- Journal of Geophysical Research, Vol. 57, Issue 2
New n-Type Zintl Phases for Thermoelectrics: Discovery, Structural Characterization, and Band Engineering of the Compounds A 2 CdP 2 (A = Sr, Ba, Eu)
journal, December 2020
- Balvanz, Adam; Qu, Jiaxing; Baranets, Sviatoslav
- Chemistry of Materials, Vol. 32, Issue 24
Competing Structural Influences in the Li Superionic Conducting Argyrodites Li 6 PS 5– x Se x Br (0 ≤ x ≤ 1) upon Se Substitution
journal, October 2018
- Bernges, Tim; Culver, Sean P.; Minafra, Nicolò
- Inorganic Chemistry, Vol. 57, Issue 21
Synthesis, Crystal and Electronic Structures, and Properties of the New Pnictide Semiconductors A 2 Cd Pn 2 ( A = Ca, Sr, Ba, Eu; Pn = P, As)
journal, September 2011
- Wang, Jian; Yang, Min; Pan, Ming-Yan
- Inorganic Chemistry, Vol. 50, Issue 17
Practical doping principles
journal, July 2003
- Zunger, Alex
- Applied Physics Letters, Vol. 83, Issue 1
All-scale hierarchical thermoelectrics: MgTe in PbTe facilitates valence band convergence and suppresses bipolar thermal transport for high performance
journal, January 2013
- Zhao, L. D.; Wu, H. J.; Hao, S. Q.
- Energy & Environmental Science, Vol. 6, Issue 11
Design of Light-Weight High-Entropy Alloys
journal, September 2016
- Feng, Rui; Gao, Michael; Lee, Chanho
- Entropy, Vol. 18, Issue 9
Band gap engineering approaches to increase InGaN/GaN LED efficiency
journal, January 2012
- Auf der Maur, M.; Lorenz, K.; Di Carlo, A.
- Optical and Quantum Electronics, Vol. 44, Issue 3-5
Cation−Anion Interactions as Structure Directing Factors: Structure and Bonding of Ca 2 CdSb 2 and Yb 2 CdSb 2
journal, April 2007
- Xia, Sheng-qing; Bobev, Svilen
- Journal of the American Chemical Society, Vol. 129, Issue 13
Convergence of Conduction Bands as a Means of Enhancing Thermoelectric Performance of -Type Solid Solutions
journal, April 2012
- Liu, Wei; Tan, Xiaojian; Yin, Kang
- Physical Review Letters, Vol. 108, Issue 16
Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency
journal, April 2019
- Hanus, Riley; Agne, Matthias T.; Rettie, Alexander J. E.
- Advanced Materials, Vol. 31, Issue 21
Distributions of phonon lifetimes in Brillouin zones
journal, March 2015
- Togo, Atsushi; Chaput, Laurent; Tanaka, Isao
- Physical Review B, Vol. 91, Issue 9
Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for ZnO and GaAs
journal, December 2008
- Lany, Stephan; Zunger, Alex
- Physical Review B, Vol. 78, Issue 23, Article No. 235104
Computationally guided discovery of thermoelectric materials
journal, August 2017
- Gorai, Prashun; Stevanović, Vladan; Toberer, Eric S.
- Nature Reviews Materials, Vol. 2, Issue 9
Defect chemistry of disordered solid-state electrolyte Li 10 GeP 2 S 12
journal, January 2020
- Gorai, Prashun; Long, Hai; Jones, Eric
- Journal of Materials Chemistry A, Vol. 8, Issue 7
First-Principles Theory of Competing Order Types, Phase Separation, and Phonon Spectra in Thermoelectric Alloys
journal, October 2008
- Barabash, S. V.; Ozolins, V.; Wolverton, C.
- Physical Review Letters, Vol. 101, Issue 15
Discovery of new materials using combinatorial synthesis and high-throughput characterization of thin-film materials libraries combined with computational methods
journal, July 2019
- Ludwig, Alfred
- npj Computational Materials, Vol. 5, Issue 1
OLEX2 : a complete structure solution, refinement and analysis program
journal, January 2009
- Dolomanov, Oleg V.; Bourhis, Luc J.; Gildea, Richard J.
- Journal of Applied Crystallography, Vol. 42, Issue 2
Multicomponent multisublattice alloys, nonconfigurational entropy and other additions to the Alloy Theoretic Automated Toolkit
journal, June 2009
- van de Walle, Axel
- Calphad, Vol. 33, Issue 2
Functionally graded shape memory alloys: Design, fabrication and experimental evaluation
journal, June 2017
- Shariat, Bashir S.; Meng, Qinglin; Mahmud, Abdus S.
- Materials & Design, Vol. 124
A simple chemical guide for finding novel n-type dopable Zintl pnictide thermoelectric materials
journal, January 2019
- Gorai, Prashun; Goyal, Anuj; Toberer, Eric S.
- Journal of Materials Chemistry A, Vol. 7, Issue 33
Phonon conduction in PbSe, PbTe, and PbTe Se from first-principles calculations
journal, May 2012
- Tian, Zhiting; Garg, Jivtesh; Esfarjani, Keivan
- Physical Review B, Vol. 85, Issue 18
Promising bulk nanostructured Cu 2 Se thermoelectrics via high throughput and rapid chemical synthesis
journal, January 2016
- Tafti, Mohsen Y.; Ballikaya, Sedat; Khachatourian, Adrine Malek
- RSC Advances, Vol. 6, Issue 112
Machine learning assisted design of high entropy alloys with desired property
journal, May 2019
- Wen, Cheng; Zhang, Yan; Wang, Changxin
- Acta Materialia, Vol. 170
A computational framework for automation of point defect calculations
journal, April 2017
- Goyal, Anuj; Gorai, Prashun; Peng, Haowei
- Computational Materials Science, Vol. 130
A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS 3 ) and related substitutions
journal, January 2017
- Faghaninia, Alireza; Yu, Guodong; Aydemir, Umut
- Physical Chemistry Chemical Physics, Vol. 19, Issue 9
Convergence of density and hybrid functional defect calculations for compound semiconductors
journal, September 2013
- Peng, Haowei; Scanlon, David O.; Stevanovic, Vladan
- Physical Review B, Vol. 88, Issue 11
Band engineering in Mg 3 Sb 2 by alloying with Mg 3 Bi 2 for enhanced thermoelectric performance
journal, January 2018
- Imasato, Kazuki; Kang, Stephen Dongmin; Ohno, Saneyuki
- Materials Horizons, Vol. 5, Issue 1
Phase Boundary Mapping to Obtain n-type Mg3Sb2-Based Thermoelectrics
journal, January 2018
- Ohno, Saneyuki; Imasato, Kazuki; Anand, Shashwat
- Joule, Vol. 2, Issue 1
Material descriptors for predicting thermoelectric performance
journal, January 2015
- Yan, Jun; Gorai, Prashun; Ortiz, Brenden
- Energy & Environmental Science, Vol. 8, Issue 3
High Thermoelectric Performance in SnTe–AgSbTe 2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence
journal, February 2018
- Tan, Gangjian; Hao, Shiqiang; Hanus, Riley C.
- ACS Energy Letters, Vol. 3, Issue 3
Syntheses, and crystal and electronic structures of the new Zintl phases Na2ACdSb2 and K2ACdSb2 (A=Ca, Sr, Ba, Eu, Yb): Structural relationship with Yb2CdSb2 and the solid solutions Sr2–xAxCdSb2, Ba2–xAxCdSb2 and Eu2–xYbxCdSb2
journal, February 2011
- Saparov, Bayrammurad; Saito, Maia; Bobev, Svilen
- Journal of Solid State Chemistry, Vol. 184, Issue 2
Enhancement of Piezoelectric Response in Scandium Aluminum Nitride Alloy Thin Films Prepared by Dual Reactive Cosputtering
journal, December 2008
- Akiyama, Morito; Kamohara, Toshihiro; Kano, Kazuhiko
- Advanced Materials, Vol. 21, Issue 5
Native Defect Engineering in CuInTe 2
journal, December 2020
- Adamczyk, Jesse M.; Gomes, Lídia C.; Qu, Jiaxing
- Chemistry of Materials, Vol. 33, Issue 1
Crystal structure refinement with SHELXL
journal, January 2015
- Sheldrick, George M.
- Acta Crystallographica Section C Structural Chemistry, Vol. 71, Issue 1, p. 3-8
First-principles calculations for point defects in solids
journal, March 2014
- Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann
- Reviews of Modern Physics, Vol. 86, Issue 1
Effects of extrinsic and intrinsic perturbations on the electronic structure of graphene: Retaining an effective primitive cell band structure by band unfolding
journal, January 2014
- Medeiros, Paulo V. C.; Stafström, Sven; Björk, Jonas
- Physical Review B, Vol. 89, Issue 4
Effective Band Structure of Random Alloys
journal, June 2010
- Popescu, Voicu; Zunger, Alex
- Physical Review Letters, Vol. 104, Issue 23
Overcoming the doping bottleneck in semiconductors
journal, August 2004
- Wei, Su-Huai
- Computational Materials Science, Vol. 30, Issue 3-4
Solid Solution Yb 2– x Ca x CdSb 2 : Structure, Thermoelectric Properties, and Quality Factor
journal, August 2021
- Devlin, Kasey P.; Chen, Shunda; Donadio, Davide
- Inorganic Chemistry, Vol. 60, Issue 17
Gapped metals as thermoelectric materials revealed by high-throughput screening
journal, January 2020
- Ricci, Francesco; Dunn, Alexander; Jain, Anubhav
- Journal of Materials Chemistry A, Vol. 8, Issue 34
Special quasirandom structures
journal, July 1990
- Zunger, Alex; Wei, S.-H.; Ferreira, L. G.
- Physical Review Letters, Vol. 65, Issue 3, p. 353-356
Doping by design: finding new n-type dopable ABX 4 Zintl phases for thermoelectrics
journal, January 2020
- Qu, Jiaxing; Stevanović, Vladan; Ertekin, Elif
- Journal of Materials Chemistry A, Vol. 8, Issue 47
Defect chemistry and doping of BiCuSeO
journal, January 2021
- Toriyama, Michael Y.; Qu, Jiaxing; Snyder, G. Jeffrey
- Journal of Materials Chemistry A, Vol. 9, Issue 36
Machine learning guided appraisal and exploration of phase design for high entropy alloys
journal, December 2019
- Zhou, Ziqing; Zhou, Yeju; He, Quanfeng
- npj Computational Materials, Vol. 5, Issue 1
Computational and experimental investigation of TmAgTe 2 and XYZ 2 compounds, a new group of thermoelectric materials identified by first-principles high-throughput screening
journal, January 2015
- Zhu, Hong; Hautier, Geoffroy; Aydemir, Umut
- Journal of Materials Chemistry C, Vol. 3, Issue 40
Exceeding 20% efficiency with in situ group V doping in polycrystalline CdTe solar cells
journal, August 2019
- Metzger, W. K.; Grover, S.; Lu, D.
- Nature Energy, Vol. 4, Issue 10
Theoretical prediction of high melting temperature for a Mo–Ru–Ta–W HCP multiprincipal element alloy
journal, January 2021
- Hong, Qi-Jun; Schroers, Jan; Hofmann, Douglas
- npj Computational Materials, Vol. 7, Issue 1
A Review on Functionally Graded Materials and Structures via Additive Manufacturing: From Multi‐Scale Design to Versatile Functional Properties
journal, April 2020
- Li, Yan; Feng, Zuying; Hao, Liang
- Advanced Materials Technologies, Vol. 5, Issue 6