Combining density functional theory calculations, supercomputing, and data-driven methods to design new thermoelectric materials
Anubhav JainEnergy Technologies Area
Lawrence Berkeley National LaboratoryBerkeley, CA
AIChE 2016
Slides posted to http://www.slideshare.net/anubhavster
Using density functional theory to design new materials
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A. Jain, Y. Shin, and K. A. Persson, Nat. Rev. Mater. 1, 15004 (2016).
We’ve initiated a search for new bulk thermoelectrics
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Initial procedure similar to Madsen (2006)
On top of this traditional procedure we add:• thermal conductivity
model of Pohl-Cahill• targeted defect
calculations to assess doping
• Today - ~50,000 compounds screened!
Madsen, G. K. H. Automated search for new thermoelectric materials: the case of LiZnSb.J. Am. Chem. Soc., 2006, 128, 12140–6
New Materials from screening – TmAgTe2 (calcs)
4Zhu, H.; Hautier, G.; Aydemir, U.; Gibbs, Z. M.; Li, G.; Bajaj, S.; Pöhls, J.-H.; Broberg, D.; Chen, W.; Jain, A.; White, M. A.; Asta, M.; Snyder, G. J.; Persson, K.; Ceder, G. Computational and experimental investigation of TmAgTe 2 and XYZ 2 compounds, a new group of thermoelectric materials identified by first-principles high-throughput screening, J. Mater. Chem. C, 2015, 3
TmAgTe2 - experiments
5Zhu, H.; Hautier, G.; Aydemir, U.; Gibbs, Z. M.; Li, G.; Bajaj, S.; Pöhls, J.-H.; Broberg, D.; Chen, W.; Jain, A.; White, M. A.; Asta, M.; Snyder, G. J.; Persson, K.; Ceder, G. Computational and experimental investigation of TmAgTe 2 and XYZ 2 compounds, a new group of thermoelectric materials identified by first-principles high-throughput screening, J. Mater. Chem. C, 2015, 3
The limitation - doping
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p=1020
VB Edge CB Edge
n=1020
1016
E-Ef (eV)
TmAgTe2600K
OurSample
• Calculations indicate TmAg defects are most likely “hole killers”.• Tm deficient samples so far not successful• Meanwhile, explore other chemistries
YCuTe2 – friendlier elements, higher zT (0.75)
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• A combination of intuition and calculations suggest to try YCuTe2
• Higher carrier concentration of ~1019
• Retains very low thermal conductivity, peak zT ~0.75
• But – unlikely to improve further
Aydemir, U.; Pöhls, J.-H.; Zhu, H.l Hautier, G.; Bajaj, S.; Gibbs, Z. M.; Chen, W.; Li, G.; Broberg, D.; Kang, S.D.; White, M. A.; Asta, M.; Ceder, G.; Persson, K.; Jain, A.; Snyder, G. J. YCuTe2: A Member of a New Class of Thermoelectric Materials with CuTe4-Based Layered Structure. J. Mat Chem C, 2016
experiment
computation
Bournonites – CuPbSbS3 and analogues
• Natural mineral• Measured thermal conductivity for
CuPbSbS3 < 1 W/m*K– Stereochemical lone pair scattering
mechanisms• Measured Seebeck coefficient in
the range of 400 µV/K• BUT electrical conductivity likely
requires improvement – can calculations help?
• Total of 320 substitutions into ABCD3 formula computed
• Experimental study is next
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Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
Variation of properties with substitution
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Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
Variation of properties with substitution
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Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
Variation of properties with substitution
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Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
Interesting compounds and effect of scattering
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Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
Defects – selenide looks slightly better than sulfide
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(a) (b)
• Multiple defects prevent n-type formation• p-type limited by SbPb defect. Situation slightly better in sulfide because VSe can help
compensate• Extrinsic defects calculations (not shown) do not provide clear paths forward
Faghaninia A., Yu G., Aydemir U., Wood M., Chen W., Rignanese G.M., Snyder J., Hautier G., Jain, A. A computational assessment of the electronic, thermoelectric, and defect properties of bournonite (CuPbSbS3) and related substitutions (submitted)
CuPbSbS3 CuPbSbSe3
Open data and software
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www.materialsproject.org
www.pymatgen.org
www.github.com/hackingmaterials/MatMethods
www.pythonhosted.org/FireWorksNote: results of 50,000 transport calcs will eventually be posted here
Poster on automating surface calculations with these tools:Automating Workflows for Surface Science and Catalysis
Joseph H. Montoya and Kristin PerssonMonday, 6:00 PM - 8:00 PM
Grand Ballroom B (Hilton)COMSEF Poster session
Thank you!
• Collaborating research groups– Jeffrey Snyder– Geoffroy Hautier– Mary Anne White– Mark Asta– Hong Zhu– Kristin Persson– Gerbrand Ceder
• Primary researchers– TmAgTe2 – Prof. Hong Zhu and Dr. Umut Aydemir– YCuTe2 – Dr. Umut Aydemir and Dr. Jan Pohls– CuPbSbS3 – Dr. Alireza Faghaninia
• NERSC computing center and staff
• Funding: U.S. Department of Energy, Basic Energy Sciences, Materials Science Division
15Slides posted to http://www.slideshare.net/anubhavster