Presentation given at the AIChE conference in San Francisco

1. Combining density functional theory calculations,
supercomputing, and data-driven methods to design
new thermoelectric materials
Anubhav Jain
Energy Technologies Area
Lawrence Berkeley National Laboratory
Berkeley, CA
AIChE 2016
Slides posted to http://www.slideshare.net/anubhavster

2. Using density functional theory to design new materials
2
A. Jain, Y. Shin, and K. A.
Persson, Nat. Rev. Mater.
1, 15004 (2016).

3. We’ve initiated a search for new bulk thermoelectrics
3
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

4. New Materials from screening – TmAgTe2 (calcs)
4
Zhu, 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

5. TmAgTe2 - experiments
5
Zhu, 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

6. The limitation - doping
6
p=1020
VB Edge CB Edge
n=1020
1016
E-Ef (eV)
TmAgTe2
600K
Our
Sample
• Calculations indicate TmAg defects are most likely “hole killers”.
• Tm deficient samples so far not successful
• Meanwhile, explore other chemistries

7. YCuTe2 – friendlier elements, higher zT (0.75)
7
• 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

8. 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
8
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)

9. Variation of properties with substitution
9
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)

10. Variation of properties with substitution
10
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)

11. Variation of properties with substitution
11
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)

12. Interesting compounds and effect of scattering
12
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)

13. Defects – selenide looks slightly better than sulfide
13
(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

14. Open data and software
14
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 Persson
Monday, 6:00 PM - 8:00 PM
Grand Ballroom B (Hilton)
COMSEF Poster session

15. 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