Accelerating Thermoelectric Materials Discovery via Dopability Predictions

The project’s ultimate objective is to build a robust and accurate dopability recommendation engine to overcome the dopability bottleneck in thermoelectric materials discovery. The recommendation engine will use materials informatics to enable high-throughput predictions of dopability, relying only on quantities that are inexpensive to calculate, experimental measurements, and known structural/chemical features as inputs. It will thus allow dopability screening of thousands of compounds. First, an accurate training set will be built for the recommendation engine containing native defect formation enthalpies and structural/chemical descriptors from a diverse array of thermoelectric-relevant compounds. Whereas prior dopant studies focused on single compounds, a new, automated calculation infrastructure will be leveraged that allows the rapid creation of an extensive training set, initially containing approximately 30 compounds but growing to over 100 during the project. Experimental charge transport and local dopant structure measurements will validate the training set. Second, the prediction engine will be trained on the data to extract patterns and correlations, and ultimately identify robust descriptors of dopability. Initially, the engine will predict if `killer' defects limit the available dopant range. The engine will ultimately grow to suggest specific extrinsic dopants for compounds that pass this initial screening. Together, this combination of accurate predictions of intrinsic transport properties (prior DMREF) and dopability (proposed DMREF) is expected to accelerate the discovery process for thermoelectric materials.

Publications

Simulating high-entropy alloys at finite temperatures: An uncertainty-based approach

A. Novick, Q. Nguyen, R. Garnett, E. Toberer, and V. Stevanović

6/5/2023

VTAnDeM: A python toolkit for simultaneously visualizing phase stability, defect energetics, and carrier concentrations of materials

M. Y. Toriyama, J. Qu, L. C. Gomes, and E. Ertekin

6/1/2023

New Zintl Phase Yb₁₀MgSb₉ with High Thermoelectric Performance

L. Borgsmiller, Q. Li, M. Y. Toriyama, and G. J. Snyder

4/7/2023

Thermoelectric Properties of Ba_2–xEu_xZnSb₂, a Zintl Phase with One-Dimensional Covalent Chains

A. K. Hauble, K. Ciesielski, V. Taufour, E. S. Toberer, and S. M. Kauzlarich

4/6/2023

Strong Scattering from Low-Frequency Rattling Modes Results in Low Thermal Conductivity in Antimonide Clathrate Compounds

K. M. Ciesielski, B. R. Ortiz, L. C. Gomes, V. Meschke, J. Adamczyk, T. L. Braden, D. Kaczorowski, E. Ertekin, and E. S. Toberer

3/22/2023

The Importance of Mg–Sb Interactions in Achieving High Conduction Band Degeneracy in Mg3Sb2 for High n-Type Thermoelectric Performance

M. K. Brod, S. Anand, and G. Jeffrey Snyder

2/1/2023

Extrinsic doping of Hg₂GeTe₄ in the face of defect compensation and phase competition

C. E. Porter, J. Qu, K. Cielsielski, E. Ertekin, and E. S. Toberer

1/1/2023

Designing for dopability in semiconducting AgInTe₂

V. Meschke, L. C. Gomes, J. M. Adamczyk, K. M. Ciesielski, C. M. Crawford, H. Vinton, E. Ertekin, and E. S. Toberer

1/1/2023

Giant phonon anharmonicity driven by the asymmetric lone pairs in Mg3Bi2

Y. Zhu, J. Liu, B. Wei, S. Xu, Y. Song, X. Wang, T. -. Xia, J. Chen, G. J. Snyder, and J. Hong

10/1/2022

Chemical Interpretation of Charged Point Defects in Semiconductors: A Case Study of Mg₂Si

M. Y. Toriyama, M. K. Brod, and G. J. Snyder

7/8/2022

Simulation and characterization of cation disorder in $$\hbox {ZnGeP}_{2}$$

J. J. Cordell, L. Pucurimay, R. R. Schnepf, B. L. Levy-Wendt, M. F. Toney, G. J. Tucker, S. Lany, and A. C. Tamboli

6/28/2022

A Convergent Understanding of Charged Defects

S. Anand, M. Y. Toriyama, C. Wolverton, S. M. Haile, and G. J. Snyder

6/21/2022

Effective Mass from Seebeck Coefficient

G. J. Snyder, A. Pereyra, and R. Gurunathan

2/9/2022

Thermodynamic Guidelines for Maximum Solubility

S. Anand, C. Wolverton, and G. J. Snyder

2/2/2022

Thermoelectric properties and low thermal conductivity of Zintl compound Yb₁₀MnSb₉

L. Borgsmiller, and G. J. Snyder

1/1/2022

Symmetry breaking in Ge_1−xMn_xTe and the impact on thermoelectric transport

J. M. Adamczyk, F. A. Bipasha, G. A. Rome, K. Ciesielski, E. Ertekin, and E. S. Toberer

1/1/2022

Conduction band engineering of half-Heusler thermoelectrics using orbital chemistry

S. Guo, S. Anand, M. K. Brod, Y. Zhang, and G. J. Snyder

1/1/2022

Tuning valley degeneracy with band inversion

M. Y. Toriyama, M. K. Brod, L. C. Gomes, F. A. Bipasha, B. A. Assaf, E. Ertekin, and G. J. Snyder

1/1/2022

Estimating the lower-limit of fracture toughness from ideal-strength calculations

L. Borgsmiller, M. T. Agne, J. P. Male, S. Anand, G. Li, S. I. Morozov, and G. J. Snyder

1/1/2022

Band Engineering SnTe via Trivalent Substitutions for Enhanced Thermoelectric Performance

X. Zhang, Z. Wang, B. Zou, M. K. Brod, J. Zhu, T. Jia, G. Tang, G. J. Snyder, and Y. Zhang

12/6/2021

Finding the order in complexity: The electronic structure of 14-1-11 zintl compounds

Y. Liu, M. Y. Toriyama, Z. Cai, M. Zhao, F. Liu, and G. Jeffrey Snyder

11/22/2021

First principles investigation of intrinsic and Na defects in XTe (X=Ca, Sr, Ba) nanostructured PbTe

X. Zhang, M. Y. Toriyama, J. P. Male, Z. Feng, S. Guo, T. Jia, Z. Ti, G. J. Snyder, and Y. Zhang

7/1/2021

Physical insights on the low lattice thermal conductivity of AgInSe2

Y. Zhu, B. Wei, J. Liu, N. Z. Koocher, Y. Li, L. Hu, W. He, G. Deng, W. Xu, X. Wang, J. M. Rondinelli, L. Zhao, G. J. Snyder, and J. Hong

7/1/2021

When band convergence is not beneficial for thermoelectrics

J. Park, M. Dylla, Y. Xia, M. Wood, G. J. Snyder, and A. Jain

6/8/2021

Quantifying charge carrier localization in chemically doped semiconducting polymers

S. A. Gregory, R. Hanus, A. Atassi, J. M. Rinehart, J. P. Wooding, A. K. Menon, M. D. Losego, G. J. Snyder, and S. K. Yee

5/20/2021

Charge-carrier-mediated lattice softening contributes to high zT in thermoelectric semiconductors

T. J. Slade, S. Anand, M. Wood, J. P. Male, K. Imasato, D. Cheikh, M. M. Al Malki, M. T. Agne, K. J. Griffith, S. K. Bux, C. Wolverton, M. G. Kanatzidis, and G. J. Snyder

5/1/2021

Phase Boundary Mapping of Tin‐Doped ZnSb Reveals Thermodynamic Route to High Thermoelectric Efficiency

M. Wood, M. Y. Toriyama, S. Dugar, J. Male, S. Anand, V. Stevanović, and G. J. Snyder

4/14/2021

Distributed and localized cooling with thermoelectrics

G. J. Snyder, S. LeBlanc, D. Crane, H. Pangborn, C. E. Forest, A. Rattner, L. Borgsmiller, and S. Priya

4/1/2021

Possibility of interstitial Na as electron donor in Yb14MgSb11

N. A. Pieczulewski, M. Wood, M. Y. Toriyama, J. P. Male, K. J. Griffith, and G. J. Snyder

2/26/2021

Anomalous electronic properties in layered, disordered ZnVSb

E. A. Bensen, K. Ciesielski, L. C. Gomes, B. R. Ortiz, J. Falke, O. Pavlosiuk, D. Weber, T. L. Braden, K. X. Steirer, D. Szymański, J. E. Goldberger, C. Kuo, C. Chen, C. Chang, L. H. Tjeng, D. Kaczorowski, E. Ertekin, and E. S. Toberer

1/27/2021

Temperature-Dependent Band Renormalization in CoSb₃ Skutterudites Due to Sb-Ring-Related Vibrations

Z. Wang, J. Xi, J. Ning, K. Guo, B. Duan, J. Luo, G. J. Snyder, J. Yang, and W. Zhang

1/25/2021

Understanding Cu incorporation in the Cu2xHg2−xGeTe4 structure using resonant x-ray diffraction

B. L. Levy-Wendt, B. R. Ortiz, L. C. Gomes, K. H. Stone, D. Passarello, E. Ertekin, E. S. Toberer, and M. F. Toney

1/15/2021

Computationally Guided Discovery of Axis-Dependent Conduction Polarity in NaSnAs Crystals

A. M. Ochs, P. Gorai, Y. Wang, M. R. Scudder, K. Koster, C. E. Moore, V. Stevanovic, J. P. Heremans, W. Windl, E. S. Toberer, and J. E. Goldberger

1/15/2021

Defect chemistry and doping of BiCuSeO

M. Y. Toriyama, J. Qu, G. J. Snyder, and P. Gorai

1/1/2021

The effect of Mg₃As₂ alloying on the thermoelectric properties of n-type Mg₃(Sb, Bi)₂

K. Imasato, S. Anand, R. Gurunathan, and G. J. Snyder

1/1/2021

Using phase boundary mapping to resolve discrepancies in the Mg₂Si–Mg₂Sn miscibility gap

R. Orenstein, J. P. Male, M. Toriyama, S. Anand, and G. J. Snyder

1/1/2021

Controlling thermoelectric transport via native defects in the diamond-like semiconductors Cu₂HgGeTe₄ and Hg₂GeTe₄

J. Qu, C. E. Porter, L. C. Gomes, J. M. Adamczyk, M. Y. Toriyama, B. R. Ortiz, E. S. Toberer, and E. Ertekin

1/1/2021

Visualizing defect energetics

S. Anand, J. P. Male, C. Wolverton, and G. J. Snyder

1/1/2021

Orbital chemistry of high valence band convergence and low-dimensional topology in PbTe

M. K. Brod, and G. J. Snyder

1/1/2021

Native Defect Engineering in CuInTe₂

J. M. Adamczyk, L. C. Gomes, J. Qu, G. A. Rome, S. M. Baumann, E. Ertekin, and E. S. Toberer

12/16/2020

New n-Type Zintl Phases for Thermoelectrics: Discovery, Structural Characterization, and Band Engineering of the Compounds A₂CdP₂ (A = Sr, Ba, Eu)

A. Balvanz, J. Qu, S. Baranets, E. Ertekin, P. Gorai, and S. Bobev

12/14/2020

Orbital Chemistry That Leads to High Valley Degeneracy in PbTe

M. K. Brod, M. Y. Toriyama, and G. J. Snyder

11/13/2020

Weighted Mobility

G. J. Snyder, A. H. Snyder, M. Wood, R. Gurunathan, B. H. Snyder, and C. Niu

5/14/2020

On the Dopability of Semiconductors and Governing Material Properties

A. Goyal, P. Gorai, S. Anand, E. S. Toberer, G. J. Snyder, and V. Stevanović

5/6/2020

Analytical Models of Phonon–Point-Defect Scattering

R. Gurunathan, R. Hanus, M. Dylla, A. Katre, and G. J. Snyder

3/4/2020

Discovery of n-Type Zintl Phases RbAlSb₄, RbGaSb₄, CsAlSb₄, and CsGaSb₄

B. R. Ortiz, P. Gorai, T. Braden, E. A. Bensen, S. D. Wilson, V. Stevanović, and E. S. Toberer

2/20/2020

Graphene/Strontium Titanate: Approaching Single Crystal–Like Charge Transport in Polycrystalline Oxide Perovskite Nanocomposites through Grain Boundary Engineering

Y. Lin, M. T. Dylla, J. J. Kuo, J. P. Male, I. A. Kinloch, R. Freer, and G. J. Snyder

2/3/2020

Using resonant energy X-ray diffraction to extract chemical order parameters in ternary semiconductors

R. R. Schnepf, B. L. Levy-Wendt, M. B. Tellekamp, B. R. Ortiz, C. L. Melamed, L. T. Schelhas, K. H. Stone, M. F. Toney, E. S. Toberer, and A. C. Tamboli

1/1/2020

Thermoelectric transport of semiconductor full-Heusler VFe₂Al

S. Anand, R. Gurunathan, T. Soldi, L. Borgsmiller, R. Orenstein, and G. J. Snyder

1/1/2020

Doping by design: finding new n-type dopable ABX₄ Zintl phases for thermoelectrics

J. Qu, V. Stevanović, E. Ertekin, and P. Gorai

1/1/2020

The importance of the Mg–Mg interaction in Mg₃Sb₂–Mg₃Bi₂ shown through cation site alloying

M. Wood, K. Imasato, S. Anand, J. Yang, and G. J. Snyder

1/1/2020

Computational discovery of promising new n-type dopable ABX Zintl thermoelectric materials

P. Gorai, A. Ganose, A. Faghaninia, A. Jain, and V. Stevanović

1/1/2020

Machine Learning Chemical Guidelines for Engineering Electronic Structures in Half-Heusler Thermoelectric Materials

M. T. Dylla, A. Dunn, S. Anand, A. Jain, and G. J. Snyder

1/1/2020

Discovery of high-performance thermoelectric copper chalcogenide using modified diffusion-couple high-throughput synthesis and automated histogram analysis technique

T. Deng, T. Xing, M. K. Brod, Y. Sheng, P. Qiu, I. Veremchuk, Q. Song, T. Wei, J. Yang, G. J. Snyder, Y. Grin, L. Chen, and X. Shi

1/1/2020

Alloy scattering of phonons

R. Gurunathan, R. Hanus, and G. J. Snyder

1/1/2020

Comment on “Understanding the Intrinsic P-Type Behavior and Phase Stability of Thermoelectric α-Mg₃Sb₂”

P. Gorai, and V. Stevanović

12/26/2019

Microstructure and composition engineering Yb single-filled CoSb3 for high thermoelectric and mechanical performances

Z. Zhou, M. T. Agne, Q. Zhang, S. Wan, Q. Song, Q. Xu, X. Lu, S. Gu, Y. Fan, W. Jiang, G. J. Snyder, and L. Wang

12/1/2019

Synergistically Optimizing Carrier Concentration and Decreasing Sound Velocity in n-type AgInSe₂ Thermoelectrics

Y. Zhu, Y. Liu, M. Wood, N. Z. Koocher, Y. Liu, L. Liu, T. Hu, J. M. Rondinelli, J. Hong, G. J. Snyder, and W. Xu

9/18/2019

New kagome prototype materials: discovery of KV3Sb5,RbV3Sb5 , and CsV3Sb5

B. R. Ortiz, L. C. Gomes, J. R. Morey, M. Winiarski, M. Bordelon, J. S. Mangum, I. W. H. Oswald, J. A. Rodriguez-Rivera, J. R. Neilson, S. D. Wilson, E. Ertekin, T. M. McQueen, and E. S. Toberer

9/16/2019

Grain Boundary Engineering Nanostructured SrTiO₃ for Thermoelectric Applications

M. T. Dylla, J. J. Kuo, I. Witting, and G. J. Snyder

5/8/2019

Double Half-Heuslers

S. Anand, M. Wood, Y. Xia, C. Wolverton, and G. J. Snyder

5/1/2019

The Thermoelectric Properties of Bismuth Telluride

I. T. Witting, T. C. Chasapis, F. Ricci, M. Peters, N. A. Heinz, G. Hautier, and G. J. Snyder

4/5/2019

Rapid Prediction of Anisotropic Lattice Thermal Conductivity: Application to Layered Materials

R. McKinney, P. Gorai, E. S. Toberer, and V. Stevanovic̀

2/15/2019

Effect of Two‐Dimensional Crystal Orbitals on Fermi Surfaces and Electron Transport in Three‐Dimensional Perovskite Oxides

M. T. Dylla, S. D. Kang, and G. J. Snyder

2/12/2019

Effective n-type doping of Mg3Sb2 with group-3 elements

P. Gorai, E. S. Toberer, and V. Stevanović

1/8/2019

Carrier density control in Cu₂HgGeTe₄and discovery of Hg₂GeTe₄viaphase boundary mapping

B. R. Ortiz, K. Gordiz, L. C. Gomes, T. Braden, J. M. Adamczyk, J. Qu, E. Ertekin, and E. S. Toberer

1/1/2019

A simple chemical guide for finding novel n-type dopable Zintl pnictide thermoelectric materials

P. Gorai, A. Goyal, E. S. Toberer, and V. Stevanović

1/1/2019

Mixed phononic and non-phononic transport in hybrid lead halide perovskites: glass-crystal duality, dynamical disorder, and anharmonicity

T. Zhu, and E. Ertekin

1/1/2019

The importance of phase equilibrium for doping efficiency: iodine doped PbTe

J. Male, M. T. Agne, A. Goyal, S. Anand, I. T. Witting, V. Stevanović, and G. J. Snyder

1/1/2019

Empirical modeling of dopability in diamond-like semiconductors

S. A. Miller, M. Dylla, S. Anand, K. Gordiz, G. J. Snyder, and E. S. Toberer

12/6/2018

The 2019 materials by design roadmap

K. Alberi, M. B. Nardelli, A. Zakutayev, L. Mitas, S. Curtarolo, A. Jain, M. Fornari, N. Marzari, I. Takeuchi, M. L. Green, M. Kanatzidis, M. F. Toney, S. Butenko, B. Meredig, S. Lany, U. Kattner, A. Davydov, E. S. Toberer, V. Stevanovic, A. Walsh, N. Park, A. Aspuru-Guzik, D. P. Tabor, J. Nelson, J. Murphy, A. Setlur, J. Gregoire, H. Li, R. Xiao, A. Ludwig, L. W. Martin, A. M. Rappe, S. Wei, and J. Perkins

10/24/2018

Temperature Dependent n‐Type Self Doping in Nominally 19‐Electron Half‐Heusler Thermoelectric Materials

S. Anand, K. Xia, T. Zhu, C. Wolverton, and G. J. Snyder

9/19/2018

Discovery of High-Performance Thermoelectric Chalcogenides through Reliable High-Throughput Material Screening

L. Xi, S. Pan, X. Li, Y. Xu, J. Ni, X. Sun, J. Yang, J. Luo, J. Xi, W. Zhu, X. Li, D. Jiang, R. Dronskowski, X. Shi, G. J. Snyder, and W. Zhang

8/8/2018

Heat capacity of Mg3Sb2, Mg3Bi2, and their alloys at high temperature

M. T. Agne, K. Imasato, S. Anand, K. Lee, S. K. Bux, A. Zevalkink, A. J. E. Rettie, D. Y. Chung, M. G. Kanatzidis, and G. J. Snyder

8/1/2018

Thermopower-conductivity relation for distinguishing transport mechanisms: Polaron hopping in CeO2 and band conduction in SrTiO3

S. D. Kang, M. Dylla, and G. J. Snyder

6/6/2018

A practical field guide to thermoelectrics: Fundamentals, synthesis, and characterization

A. Zevalkink, D. M. Smiadak, J. L. Blackburn, A. J. Ferguson, M. L. Chabinyc, O. Delaire, J. Wang, K. Kovnir, J. Martin, L. T. Schelhas, T. D. Sparks, S. D. Kang, M. T. Dylla, G. J. Snyder, B. R. Ortiz, and E. S. Toberer

6/1/2018

Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects

B. R. Ortiz, W. Peng, L. C. Gomes, P. Gorai, T. Zhu, D. M. Smiadak, G. J. Snyder, V. Stevanović, E. Ertekin, A. Zevalkink, and E. S. Toberer

5/2/2018

Investigation of n-type doping strategies for Mg₃Sb₂

P. Gorai, B. R. Ortiz, E. S. Toberer, and V. Stevanović

1/1/2018

First-principles calculations and experimental studies of XYZ₂ thermoelectric compounds: detailed analysis of van der Waals interactions

J. Pöhls, Z. Luo, U. Aydemir, J. Sun, S. Hao, J. He, I. G. Hill, G. Hautier, A. Jain, X. Zeng, C. Wolverton, G. J. Snyder, H. Zhu, and M. A. White

1/1/2018

Experimental and computational phase boundary mapping of Co₄Sn₆Te₆

C. Crawford, B. R. Ortiz, P. Gorai, V. Stevanovic, and E. S. Toberer