Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics

Perriot, Romain; Uberuaga, Blas P.; Zamora, Richard J.; Perez, Danny; Voter, Arthur F.

doi:10.1038/s41467-017-00708-z

Title: Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics

Journal Article · Wed Sep 20 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-00708-z· OSTI ID:1402615

^[1];

^[1]; Zamora, Richard J. ^[1]; Perez, Danny ^[1]; Voter, Arthur F. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Diffusion in complex oxides is critical to ionic transport, radiation damage evolution, sintering, and aging. In complex oxides such as pyrochlores, anionic diffusion is dramatically affected by cation disorder. However, little is known about how disorder influences cation transport. Here, we report results from classical and accelerated molecular dynamics simulations of vacancy-mediated cation diffusion in Gd₂Ti₂O₇ pyrochlore, on the microsecond timescale. We find that diffusion is slow at low levels of disorder, while higher disorder allows for fast diffusion, which is then accompanied by antisite annihilation and reordering, and thus a slowing of cation transport. Cation diffusivity is therefore not constant, but decreases as the material reorders. We also show that fast cation diffusion is triggered by the formation of a percolation network of antisites. This is in contrast with observations from other complex oxides and disordered media models, suggesting a fundamentally different relation between disorder and mass transport.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); LANL Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1402615

Report Number(s):: LA-UR-16-25519

Journal Information:: Nature Communications, Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 18 works

Citation information provided by
Web of Science

References (60)

Connection between oxygen-ion conductivity of pyrochlore fuel-cell materials and structural change with composition and temperature Wuensch, B. Solid State Ionics, Vol. 129, Issue 1-4 https://doi.org/10.1016/S0167-2738(99)00320-3	journal	April 2000
Diffusion Coefficients of Single and Many Particles in Lattices with Different Forms of Disorder Kehr, K. W.; Wichmann, T. Materials Science Forum, Vol. 223-224 https://doi.org/10.4028/www.scientific.net/MSF.223-224.151	journal	July 1996
Effect of Cation Ordering on Oxygen Vacancy Diffusion Pathways in Double Perovskites Uberuaga, Blas Pedro; Pilania, Ghanshyam Chemistry of Materials, Vol. 27, Issue 14 https://doi.org/10.1021/acs.chemmater.5b01474	journal	July 2015
Erratum: Percolation thresholds and universal formulas [Phys. Rev. E 55, 1514 (1997)] van der Marck, S. C. Physical Review E, Vol. 56, Issue 3 https://doi.org/10.1103/physreve.56.3732.2	journal	September 1997
Hierarchical MnMoO4/CoMoO4 heterostructured nanowires with enhanced supercapacitor performance Mai, Li-Qiang; Yang, Fan; Zhao, Yun-Long Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1387	journal	July 2011
Achieving fast oxygen diffusion in perovskites by cation ordering Taskin, A. A.; Lavrov, A. N.; Ando, Yoichi Applied Physics Letters, Vol. 86, Issue 9 https://doi.org/10.1063/1.1864244	journal	February 2005
Prediction of Rare-Earth A ₂ Hf ₂ O ₇ Pyrochlore Phases Stanek, Christopher R.; Grimes, Robin W. Journal of the American Ceramic Society, Vol. 85, Issue 8 https://doi.org/10.1111/j.1151-2916.2002.tb00423.x	journal	August 2002
Radiation effects in nuclear waste forms for high-level radioactive waste Ewing, R. C.; Weber, W. J.; Clinard, F. W. Progress in Nuclear Energy, Vol. 29, Issue 2 https://doi.org/10.1016/0149-1970(94)00016-Y	journal	January 1995
Recent advances in percolation theory and its applications Saberi, Abbas Ali arXiv https://doi.org/10.48550/arxiv.1504.02898	text	January 2015
Percolation thresholds and universal formulas van der Marck, S. C. Physical Review E, Vol. 55, Issue 2 https://doi.org/10.1103/PhysRevE.55.1514	journal	February 1997
Tunability of structure from ordered to disordered and its impact on ionic conductivity behavior in the Nd2−yHoyZr2O7 (0.0 ≤ y ≤ 2.0) system Sayed, Farheen N.; Jain, Dheeraj; Mandal, B. P. RSC Advances, Vol. 2, Issue 22 https://doi.org/10.1039/c2ra20458d	journal	January 2012
Molecular dynamics study of the effect of doping and disorder on diffusion in gadolinium zirconate Wilde, P. Solid State Ionics, Vol. 112, Issue 3-4 https://doi.org/10.1016/s0167-2738(97)00509-2	journal	October 1998
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
The incorporation of plutonium in lanthanum zirconate pyrochlore Gregg, Daniel J.; Zhang, Yingjie; Middleburgh, Simon C. Journal of Nuclear Materials, Vol. 443, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.07.030	journal	November 2013
Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries Lee, J.; Urban, A.; Li, X. Science, Vol. 343, Issue 6170 https://doi.org/10.1126/science.1246432	journal	January 2014
Long-Time Dynamics through Parallel Trajectory Splicing Perez, Danny; Cubuk, Ekin D.; Waterland, Amos Journal of Chemical Theory and Computation, Vol. 12, Issue 1 https://doi.org/10.1021/acs.jctc.5b00916	journal	December 2015
The parallel replica dynamics method – Coming of age Perez, Danny; Uberuaga, Blas P.; Voter, Arthur F. Computational Materials Science, Vol. 100 https://doi.org/10.1016/j.commatsci.2014.12.011	journal	April 2015
Ideal sinks are not always ideal: Radiation damage accumulation in nanocomposites Uberuaga, Blas Pedro; Choudhury, Samrat; Caro, Alfredo Journal of Nuclear Materials, Vol. 462 https://doi.org/10.1016/j.jnucmat.2014.11.073	journal	July 2015
Opposite correlations between cation disordering and amorphization resistance in spinels versus pyrochlores Uberuaga, Blas Pedro; Tang, Ming; Jiang, Chao Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9750	journal	October 2015
Role of Antisite Disorder on Preamorphization Swelling in Titanate Pyrochlores Li, Y. H.; Uberuaga, B. P.; Jiang, C. Physical Review Letters, Vol. 108, Issue 19 https://doi.org/10.1103/physrevlett.108.195504	journal	May 2012
Sintering of Fine Oxide Powders: II, Sintering Mechanisms Chen, Pei-Lin; Chen, I-Wei Journal of the American Ceramic Society, Vol. 80, Issue 3 https://doi.org/10.1111/j.1151-2916.1997.tb02879.x	journal	March 1997
Atomic disorder in Gd ₂ Zr ₂ O ₇ pyrochlore Zhang, F. X.; Lang, M.; Ewing, R. C. Applied Physics Letters, Vol. 106, Issue 19 https://doi.org/10.1063/1.4921268	journal	May 2015
Extending the Time Scale in Atomistic Simulation of Materials Voter, Arthur F.; Montalenti, Francesco; Germann, Timothy C. Annual Review of Materials Research, Vol. 32, Issue 1 https://doi.org/10.1146/annurev.matsci.32.112601.141541	journal	August 2002
Grain boundary stoichiometry and interactions with defects in SrTiO3 Uberuaga, Blas P.; Choudhury, Samrat; Bai, Xian-Ming Scripta Materialia, Vol. 66, Issue 2 https://doi.org/10.1016/j.scriptamat.2011.10.019	journal	January 2012
Radiation Tolerance of Complex Oxides Sickafus, K. E. Science, Vol. 289, Issue 5480 https://doi.org/10.1126/science.289.5480.748	journal	August 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
Ionic conduction in the Gd2Ti2O7−Gd2Zr2O7 system Moon, P. K.; Tuller, H. L. Solid State Ionics, Vol. 28-30 https://doi.org/10.1016/S0167-2738(88)80085-7	journal	September 1988
Structure and Mobility of Defects Formed from Collision Cascades in MgO Uberuaga, B. P.; Smith, R.; Cleave, A. R. Physical Review Letters, Vol. 92, Issue 11 https://doi.org/10.1103/physrevlett.92.115505	journal	March 2004
Frequency factors and isotope effects in solid state rate processes Vineyard, George H. Journal of Physics and Chemistry of Solids, Vol. 3, Issue 1-2 https://doi.org/10.1016/0022-3697(57)90059-8	journal	January 1957
Precise determination of the bond percolation thresholds and finite-size scaling corrections for the sc, fcc, and bcc lattices Lorenz, Christian D.; Ziff, Robert M. Physical Review E, Vol. 57, Issue 1, p. 230-236 https://doi.org/10.1103/PhysRevE.57.230	journal	January 1998
Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium Weber, W. J.; Ewing, R. C.; Catlow, C. R. A. Journal of Materials Research, Vol. 13, Issue 6 https://doi.org/10.1557/JMR.1998.0205	journal	June 1998
A new class of high capacity cation-disordered oxides for rechargeable lithium batteries: Li–Ni–Ti–Mo oxides Lee, Jinhyuk; Seo, Dong-Hwa; Balasubramanian, Mahalingam Energy & Environmental Science, Vol. 8, Issue 11 https://doi.org/10.1039/C5EE02329G	journal	January 2015
Molecular dynamics studies of radiation induced phase transitions in La2Zr2O7 pyrochlore Crocombette, Jean-Paul; Chartier, Alain Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 255, Issue 1 https://doi.org/10.1016/j.nimb.2006.11.019	journal	February 2007
Materials for Solid Oxide Fuel Cells ^† Jacobson, Allan J. Chemistry of Materials, Vol. 22, Issue 3 https://doi.org/10.1021/cm902640j	journal	February 2010
Probing disorder in isometric pyrochlore and related complex oxides Shamblin, Jacob; Feygenson, Mikhail; Neuefeind, Joerg Nature Materials, Vol. 15, Issue 5 https://doi.org/10.1038/nmat4581	journal	February 2016
Nanoionics-based resistive switching memories Waser, Rainer; Aono, Masakazu Nature Materials, Vol. 6, Issue 11, p. 833-840 https://doi.org/10.1038/nmat2023	journal	November 2007
Structural vs. intrinsic carriers: contrasting effects of cation chemistry and disorder on ionic conductivity in pyrochlores Perriot, Romain; Uberuaga, Blas P. Journal of Materials Chemistry A, Vol. 3, Issue 21 https://doi.org/10.1039/c5ta01692d	journal	January 2015
Theoretical and experimental investigation of defect formation / migration in Gd ₂ Ti ₂ O ₇ : General rule of oxide-ion migration in A ₂ B ₂ O ₇ pyrochlore Nakamura, Kaoru; Mori, Masashi; Itoh, Takanori. AIP Advances, Vol. 6, Issue 11 https://doi.org/10.1063/1.4967211	journal	November 2016
Oxygen ion conduction and structural disorder in conductive oxides Tuller, Harry L. Journal of Physics and Chemistry of Solids, Vol. 55, Issue 12 https://doi.org/10.1016/0022-3697(94)90566-5	journal	December 1994
Disorder in Pyrochlore Oxides Minervini, Licia; Grimes, Robin W.; Sickafus, Kurt E. Journal of the American Ceramic Society, Vol. 83, Issue 8 https://doi.org/10.1111/j.1151-2916.2000.tb01484.x	journal	August 2000
Strain-induced room-temperature ferroelectricity in SrTiO3 membranes Xu, Ruijuan; Huang, Jiawei; Barnard, Edward S. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16912-3	journal	June 2020
Fast-Ion Conducting Y2(Zr Ti1-)2O7 Pyrochlores: Neutron Rietveld Analysis of Disorder Induced by Zr Substitution Heremans, Catherine; Wuensch, Bernhardt J.; Stalick, Judith K. Journal of Solid State Chemistry, Vol. 117, Issue 1 https://doi.org/10.1006/jssc.1995.1253	journal	June 1995
Molecular Dynamic Simulation of Disorder Induced Amorphization in Pyrochlore Chartier, A.; Meis, C.; Crocombette, J. -P. Physical Review Letters, Vol. 94, Issue 2 https://doi.org/10.1103/PhysRevLett.94.025505	journal	January 2005
Radiation tolerance of ceramics—insights from atomistic simulation of damage accumulation in pyrochlores Devanathan, Ram; Weber, William J.; Gale, Julian D. Energy & Environmental Science, Vol. 3, Issue 10 https://doi.org/10.1039/c0ee00066c	journal	January 2010
Role of cation choice in the radiation tolerance of pyrochlores Devanathan, Ram; Gao, Fei; Sundgren, Christina J. RSC Advances, Vol. 3, Issue 9 https://doi.org/10.1039/c2ra22745b	journal	January 2013
Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides Ewing, Rodney C.; Weber, William J.; Lian, Jie Journal of Applied Physics, Vol. 95, Issue 11 https://doi.org/10.1063/1.1707213	journal	June 2004
Recent advances in percolation theory and its applications Saberi, Abbas Ali Physics Reports, Vol. 578 https://doi.org/10.1016/j.physrep.2015.03.003	journal	May 2015
Predicted pyrochlore to fluorite disorder temperature for A ₂ Zr ₂ O ₇ compositions Rushton, M. J. D.; Grimes, Robin W.; Stanek, C. R. Journal of Materials Research, Vol. 19, Issue 6 https://doi.org/10.1557/JMR.2004.0231	journal	June 2004
Key Role of the Cation Interstitial Structure in the Radiation Resistance of Pyrochlores Chartier, Alain; Catillon, Gilles; Crocombette, Jean-Paul Physical Review Letters, Vol. 102, Issue 15 https://doi.org/10.1103/PhysRevLett.102.155503	journal	April 2009
Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides Sickafus, Kurt E.; Grimes, Robin W.; Valdez, James A. Nature Materials, Vol. 6, Issue 3 https://doi.org/10.1038/nmat1842	journal	February 2007
Insights into dynamic processes of cations in pyrochlores and other complex oxides Uberuaga, Blas Pedro; Perriot, Romain Physical Chemistry Chemical Physics, Vol. 17, Issue 37 https://doi.org/10.1039/C5CP03372A	journal	January 2015
The role of surfaces, chemical interfaces, and disorder on plutonium incorporation in pyrochlores Perriot, Romain; Dholabhai, Pratik P.; Uberuaga, Blas P. Physical Chemistry Chemical Physics, Vol. 18, Issue 33 https://doi.org/10.1039/c6cp03543d	journal	January 2016
The effects of cation–anion clustering on defect migration in MgAl ₂ O ₄ Zamora, Richard J.; Voter, Arthur F.; Perez, Danny Physical Chemistry Chemical Physics, Vol. 18, Issue 29 https://doi.org/10.1039/c6cp03931f	journal	January 2016
Oxygen ion diffusion in cation ordered/disordered GdBaCo ₂ O ₅ ₊ δ Parfitt, David; Chroneos, Alexander; Tarancón, Albert J. Mater. Chem., Vol. 21, Issue 7 https://doi.org/10.1039/C0JM02924F	journal	January 2011
Advances, aging mechanisms and lifetime in solid-oxide fuel cells Tu, Hengyong; Stimming, Ulrich Journal of Power Sources, Vol. 127, Issue 1-2 https://doi.org/10.1016/j.jpowsour.2003.09.025	journal	March 2004
Parallel replica method for dynamics of infrequent events Voter, Arthur F. Physical Review B, Vol. 57, Issue 22 https://doi.org/10.1103/PhysRevB.57.R13985	journal	June 1998
Single-ion tracks in ${Gd}_{2} {Zr}_{2 - x} {Ti}_{x} O_{7}$ pyrochlores irradiated with swift heavy ions Lang, Maik; Lian, Jie; Zhang, Jiaming Physical Review B, Vol. 79, Issue 22 https://doi.org/10.1103/PhysRevB.79.224105	journal	June 2009
Nanoscale Manipulation of Pyrochlore: New Nanocomposite Ionic Conductors Lian, J.; Wang, L. M.; Wang, S. X. Physical Review Letters, Vol. 87, Issue 14 https://doi.org/10.1103/PhysRevLett.87.145901	journal	September 2001
Natural Pyrochlores: Analogues For Actinide Host Phases in Radioactive Waste Forms Lumpkin, Gregory R.; Ewing, Rodney C. MRS Proceedings, Vol. 44 https://doi.org/10.1557/PROC-44-647	journal	January 1984
Diffusion and transformation kinetics of small helium clusters in bulk tungsten Perez, Danny; Vogel, Thomas; Uberuaga, Blas P. Physical Review B, Vol. 90, Issue 1 https://doi.org/10.1103/PhysRevB.90.014102	journal	July 2014

Cited By (2)

Thermodynamic anomalies and three distinct liquid-liquid transitions in warm dense liquid hydrogen Geng, Hua Y.; Wu, Q.; Marqués, Miriam Physical Review B, Vol. 100, Issue 13 https://doi.org/10.1103/physrevb.100.134109	journal	October 2019
The impact of chemical order on defect transport in mixed pyrochlores Uberuaga, Blas P.; Perriot, Romain; Pilania, Ghanshyam Physical Chemistry Chemical Physics, Vol. 21, Issue 11 https://doi.org/10.1039/c8cp07597b	journal	January 2019

Similar Records

Structural vs. intrinsic carriers: contrasting effects of cation chemistry and disorder on ionic conductivity in pyrochlores

Journal Article · Tue Apr 21 00:00:00 EDT 2015 · Journal of Materials Chemistry. A · OSTI ID:1402615

Perriot, Romain; Uberuaga, Blas P.

Decoding ionic conductivity and reordering in cation-disordered pyrochlores

Journal Article · Mon Oct 11 00:00:00 EDT 2021 · Philosophical Transactions of the Royal Society. A, Mathematical, Physical and Engineering Sciences · OSTI ID:1402615

Annamareddy, Ajay; Eapen, Jacob

Insights into dynamic processes of cations in pyrochlores and other complex oxides

Journal Article · Wed Aug 26 00:00:00 EDT 2015 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:1402615

Uberuaga, Blas Pedro; Perriot, Romain

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
Material Science

Title: Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics

Citation Formats

References (60)

Cited By (2)

Similar Records

Related Subjects