Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores
Abstract
Structure-property relationships are a key materials science concept that enables the design of new materials. In the case of materials for application in radiation environments, correlating radiation tolerance with fundamental structural features of a material enables materials discovery. Here, we use a machine learning model to examine the factors that govern amorphization resistance in the complex oxide pyrochlore (A2B2O7) in a regime in which amorphization occurs as a consequence of defect accumulation. We examine the fidelity of predictions based on cation radii and electronegativities, the oxygen positional parameter, and the energetics of disordering and amorphizing the material. No one factor alone adequately predicts amorphization resistance. We find that when multiple families of pyrochlores (with different B cations) are considered, radii and electronegativities provide the best prediction, but when the machine learning model is restricted to only the B = Ti pyrochlores, the energetics of disordering and amorphization are critical factors. We discuss how these static quantities provide insight into an inherently kinetic property such as amorphization resistance at finite temperature. This work provides new insight into the factors that govern the amorphization susceptibility and highlights the ability of machine learning approaches to generate that insight.
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC). Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1348946
- Alternate Identifier(s):
- OSTI ID: 1361477; OSTI ID: 1508075
- Report Number(s):
- LA-UR-16-23806
Journal ID: ISSN 0897-4756
- Grant/Contract Number:
- AC52-06NA25396; EP/L005581/1; EP/L006170/1
- Resource Type:
- Published Article
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Name: Chemistry of Materials Journal Volume: 29 Journal Issue: 6; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Pilania, Ghanshyam, Whittle, Karl R., Jiang, Chao, Grimes, Robin W., Stanek, Christopher R., Sickafus, Kurt E., and Uberuaga, Blas Pedro. Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.6b04666.
Pilania, Ghanshyam, Whittle, Karl R., Jiang, Chao, Grimes, Robin W., Stanek, Christopher R., Sickafus, Kurt E., & Uberuaga, Blas Pedro. Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores. United States. https://doi.org/10.1021/acs.chemmater.6b04666
Pilania, Ghanshyam, Whittle, Karl R., Jiang, Chao, Grimes, Robin W., Stanek, Christopher R., Sickafus, Kurt E., and Uberuaga, Blas Pedro. Fri .
"Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores". United States. https://doi.org/10.1021/acs.chemmater.6b04666.
@article{osti_1348946,
title = {Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores},
author = {Pilania, Ghanshyam and Whittle, Karl R. and Jiang, Chao and Grimes, Robin W. and Stanek, Christopher R. and Sickafus, Kurt E. and Uberuaga, Blas Pedro},
abstractNote = {Structure-property relationships are a key materials science concept that enables the design of new materials. In the case of materials for application in radiation environments, correlating radiation tolerance with fundamental structural features of a material enables materials discovery. Here, we use a machine learning model to examine the factors that govern amorphization resistance in the complex oxide pyrochlore (A2B2O7) in a regime in which amorphization occurs as a consequence of defect accumulation. We examine the fidelity of predictions based on cation radii and electronegativities, the oxygen positional parameter, and the energetics of disordering and amorphizing the material. No one factor alone adequately predicts amorphization resistance. We find that when multiple families of pyrochlores (with different B cations) are considered, radii and electronegativities provide the best prediction, but when the machine learning model is restricted to only the B = Ti pyrochlores, the energetics of disordering and amorphization are critical factors. We discuss how these static quantities provide insight into an inherently kinetic property such as amorphization resistance at finite temperature. This work provides new insight into the factors that govern the amorphization susceptibility and highlights the ability of machine learning approaches to generate that insight.},
doi = {10.1021/acs.chemmater.6b04666},
journal = {Chemistry of Materials},
number = 6,
volume = 29,
place = {United States},
year = {Fri Mar 03 00:00:00 EST 2017},
month = {Fri Mar 03 00:00:00 EST 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.chemmater.6b04666
https://doi.org/10.1021/acs.chemmater.6b04666
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 28 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
From Organized High-Throughput Data to Phenomenological Theory using Machine Learning: The Example of Dielectric Breakdown
journal, February 2016
- Kim, Chiho; Pilania, Ghanshyam; Ramprasad, Ramamurthy
- Chemistry of Materials, Vol. 28, Issue 5
X-ray diffraction study of the Y2Ti2O7 pyrochlore disordering sequence under irradiation
journal, November 2016
- Soulié, Aurélien; Menut, Denis; Crocombette, Jean-Paul
- Journal of Nuclear Materials, Vol. 480
Finding Density Functionals with Machine Learning
journal, June 2012
- Snyder, John C.; Rupp, Matthias; Hansen, Katja
- Physical Review Letters, Vol. 108, Issue 25
Ion irradiation-induced phase transformation of pyrochlore and zirconolite
journal, January 1999
- Wang, S. X.; Wang, L. M.; Ewing, R. C.
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 148, Issue 1-4
An introduction to kernel-based learning algorithms
journal, March 2001
- Muller, K. -R.; Mika, S.; Ratsch, G.
- IEEE Transactions on Neural Networks, Vol. 12, Issue 2
Accelerated materials property predictions and design using motif-based fingerprints
journal, July 2015
- Huan, Tran Doan; Mannodi-Kanakkithodi, Arun; Ramprasad, Rampi
- Physical Review B, Vol. 92, Issue 1
Ion Beam-Induced Amorphization of the Pyrochlore Structure-Type: A Review
journal, January 2003
- Ewing, R. C.; Lian, J.; Wang, L. M.
- MRS Proceedings, Vol. 792
Heavy-ion irradiation effects on structures and acid dissolution of pyrochlores
journal, February 2001
- Begg, B. D.; Hess, N. J.; Weber, W. J.
- Journal of Nuclear Materials, Vol. 288, Issue 2-3
Ion-beam irradiation of Gd 2 Sn 2 O 7 and Gd 2 Hf 2 O 7 pyrochlore: Bond-type effect
journal, May 2004
- Lian, Jie; Ewing, Rodney C.; Wang, L. M.
- Journal of Materials Research, Vol. 19, Issue 5
Cation disorder in Mg O ( = Al, Ga, In) spinels from first principles
journal, July 2012
- Jiang, Chao; Sickafus, Kurt E.; Stanek, Christopher R.
- Physical Review B, Vol. 86, Issue 2
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Criteria for bombardment-induced structural changes in non-metallic solids
journal, January 1975
- Naguib, H. M.; Kelly, Roger
- Radiation Effects, Vol. 25, Issue 1
Structural stability of Nd2Zr2O7 pyrochlore ion-irradiated in a broad energy range
journal, October 2013
- Sattonnay, G.; Sellami, N.; Thomé, L.
- Acta Materialia, Vol. 61, Issue 17
Further considerations on the thermodynamics of chemical equilibria and reaction rates
journal, January 1936
- Evans, M. G.; Polanyi, M.
- Transactions of the Faraday Society, Vol. 32
Role of Antisite Disorder on Preamorphization Swelling in Titanate Pyrochlores
journal, May 2012
- Li, Y. H.; Uberuaga, B. P.; Jiang, C.
- Physical Review Letters, Vol. 108, Issue 19
Opposite correlations between cation disordering and amorphization resistance in spinels versus pyrochlores
journal, October 2015
- Uberuaga, Blas Pedro; Tang, Ming; Jiang, Chao
- Nature Communications, Vol. 6, Issue 1
Adaptive machine learning framework to accelerate ab initio molecular dynamics
journal, December 2014
- Botu, Venkatesh; Ramprasad, Rampi
- International Journal of Quantum Chemistry, Vol. 115, Issue 16
Radiation-induced amorphization of rare-earth titanate pyrochlores
journal, October 2003
- Lian, Jie; Chen, Jian; Wang, L. M.
- Physical Review B, Vol. 68, Issue 13
Radiation Tolerance of Complex Oxides
journal, August 2000
- Sickafus, K. E.
- Science, Vol. 289, Issue 5480
Machine Learning Assisted Predictions of Intrinsic Dielectric Breakdown Strength of ABX 3 Perovskites
journal, June 2016
- Kim, Chiho; Pilania, Ghanshyam; Ramprasad, Rampi
- The Journal of Physical Chemistry C, Vol. 120, Issue 27
Amorphization and recrystallization of the ABO3 oxides
journal, February 2002
- Meldrum, A.; Boatner, L. A.; Weber, W. J.
- Journal of Nuclear Materials, Vol. 300, Issue 2-3
Introduction to mathematical models for irradiation-induced phase transformations
book, January 2007
- Sickafus, Kurt E.
- Radiation Effects in Solids
The theory of reactions involving proton transfers
journal, April 1936
- Bell, Ronald Percy
- Proceedings of the Royal Society of London. Series A - Mathematical and Physical Sciences, Vol. 154, Issue 882, p. 414-429
Structural modifications in pyrochlores caused by ions in the electronic stopping regime
journal, October 2008
- Patel, M. K.; Vijayakumar, V.; Kailas, S.
- Journal of Nuclear Materials, Vol. 380, Issue 1-3
Ion irradiation of novel yttrium/ytterbium-based pyrochlores: The effect of disorder
journal, December 2011
- Whittle, Karl R.; Blackford, Mark G.; Aughterson, Robert D.
- Acta Materialia, Vol. 59, Issue 20
First-principles prediction of disordering tendencies in pyrochlore oxides
journal, March 2009
- Jiang, Chao; Stanek, C. R.; Sickafus, K. E.
- Physical Review B, Vol. 79, Issue 10
Probing disorder in isometric pyrochlore and related complex oxides
journal, February 2016
- Shamblin, Jacob; Feygenson, Mikhail; Neuefeind, Joerg
- Nature Materials, Vol. 15, Issue 5
Correlation of Formation Enthalpies with Critical Amorphization Temperature for Pyrochlore and Monazite
journal, January 2004
- Helean, K. B.; Navrotsky, A.; Lian, J.
- MRS Proceedings, Vol. 824
Fast and Accurate Modeling of Molecular Atomization Energies with Machine Learning
journal, January 2012
- Rupp, Matthias; Tkatchenko, Alexandre; Müller, Klaus-Robert
- Physical Review Letters, Vol. 108, Issue 5
Accelerating materials property predictions using machine learning
journal, September 2013
- Pilania, Ghanshyam; Wang, Chenchen; Jiang, Xun
- Scientific Reports, Vol. 3, Issue 1
The order–disorder transition in ion-irradiated pyrochlore
journal, March 2003
- Lian, J.; Wang, L.; Chen, J.
- Acta Materialia, Vol. 51, Issue 5
Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation
journal, August 2016
- Tracy, Cameron L.; Shamblin, Jacob; Park, Sulgiye
- Physical Review B, Vol. 94, Issue 6
Disorder in Pyrochlore Oxides
journal, August 2000
- Minervini, Licia; Grimes, Robin W.; Sickafus, Kurt E.
- Journal of the American Ceramic Society, Vol. 83, Issue 8
Accelerated search for materials with targeted properties by adaptive design
journal, April 2016
- Xue, Dezhen; Balachandran, Prasanna V.; Hogden, John
- Nature Communications, Vol. 7, Issue 1
Ion Irradiation of Ternary Pyrochlore Oxides
journal, July 2009
- Lumpkin, Gregory R.; Smith, Katherine L.; Blackford, Mark G.
- Chemistry of Materials, Vol. 21, Issue 13
Machine learning bandgaps of double perovskites
journal, January 2016
- Pilania, G.; Mannodi-Kanakkithodi, A.; Uberuaga, B. P.
- Scientific Reports, Vol. 6, Issue 1
Nature of the chemical bond and prediction of radiation tolerance in pyrochlore and defect fluorite compounds
journal, April 2007
- Lumpkin, Gregory R.; Pruneda, Miguel; Rios, Susana
- Journal of Solid State Chemistry, Vol. 180, Issue 4
Effect of Structure and Thermodynamic Stability on the Response of Lanthanide Stannate Pyrochlores to Ion Beam Irradiation
journal, February 2006
- Lian, J.; Helean, K. B.; Kennedy, B. J.
- The Journal of Physical Chemistry B, Vol. 110, Issue 5
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Defect formation energies in A 2 B 2 O 7 pyrochlores
journal, October 2015
- Li, Yan; Kowalski, Piotr M.; Beridze, George
- Scripta Materialia, Vol. 107
Learning scheme to predict atomic forces and accelerate materials simulations
journal, September 2015
- Botu, V.; Ramprasad, R.
- Physical Review B, Vol. 92, Issue 9
Key Role of the Cation Interstitial Structure in the Radiation Resistance of Pyrochlores
journal, April 2009
- Chartier, Alain; Catillon, Gilles; Crocombette, Jean-Paul
- Physical Review Letters, Vol. 102, Issue 15
Big Data of Materials Science: Critical Role of the Descriptor
journal, March 2015
- Ghiringhelli, Luca M.; Vybiral, Jan; Levchenko, Sergey V.
- Physical Review Letters, Vol. 114, Issue 10
Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides
journal, February 2007
- Sickafus, Kurt E.; Grimes, Robin W.; Valdez, James A.
- Nature Materials, Vol. 6, Issue 3
Machine Learning Strategy for Accelerated Design of Polymer Dielectrics
journal, February 2016
- Mannodi-Kanakkithodi, Arun; Pilania, Ghanshyam; Huan, Tran Doan
- Scientific Reports, Vol. 6, Issue 1
Formation enthalpies of rare earth titanate pyrochlores
journal, June 2004
- Helean, K. B.; Ushakov, S. V.; Brown, C. E.
- Journal of Solid State Chemistry, Vol. 177, Issue 6
Predicted structure and stability of -phase compositions
journal, November 2009
- Stanek, C. R.; Jiang, C.; Uberuaga, B. P.
- Physical Review B, Vol. 80, Issue 17
Special quasirandom structures
journal, July 1990
- Zunger, Alex; Wei, S.-H.; Ferreira, L. G.
- Physical Review Letters, Vol. 65, Issue 3, p. 353-356
Heavy-ion irradiation effects in Gd2(Ti2−xZrx)O7 pyrochlores
journal, February 2001
- Begg, B. D.; Hess, N. J.; McCready, D. E.
- Journal of Nuclear Materials, Vol. 289, Issue 1-2
Kernel methods in machine learning
journal, June 2008
- Hofmann, Thomas; Schölkopf, Bernhard; Smola, Alexander J.
- The Annals of Statistics, Vol. 36, Issue 3
Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides
journal, June 2004
- Ewing, Rodney C.; Weber, William J.; Lian, Jie
- Journal of Applied Physics, Vol. 95, Issue 11
Immobilisation of high level nuclear reactor wastes in SYNROC
journal, March 1979
- Ringwood, A. E.; Kesson, S. E.; Ware, N. G.
- Nature, Vol. 278, Issue 5701
Molecular dynamics simulation of displacement cascades in Cu and Ni: Thermal spike behavior
journal, June 1989
- de la Rubia, T. Diaz; Averback, R. S.; Hsieh, Horngming
- Journal of Materials Research, Vol. 4, Issue 3
Thermal spike model in the electronic stopping power regime
journal, March 1993
- Toulemonde, M.; Paumier, E.; Dufour, C.
- Radiation Effects and Defects in Solids, Vol. 126, Issue 1-4
Thermal spike recrystallisation: Molecular dynamics simulation of radiation damage in polymorphs of titania
journal, June 2008
- Marks, N. A.; Thomas, B. S.; Smith, K. L.
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 266, Issue 12-13