Structure and Mobility of Dissociated Vacancies at Twist Grain Boundaries and Screw Dislocations in Ionic Rocksalt Compounds

Kolluri, Kedarnath; Martinez Saez, Enrique; Uberuaga, Blas Pedro

doi:10.1021/acs.chemmater.7b05172

Title: Structure and Mobility of Dissociated Vacancies at Twist Grain Boundaries and Screw Dislocations in Ionic Rocksalt Compounds

Journal Article · 04 March 2018 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.7b05172 · OSTI ID:1438122

Kolluri, Kedarnath ^[1];

^[1];

^[1]

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

Interfaces, grain boundaries, and dislocations are known to have significant impact on the transport properties of materials. Even so, it is still not clear how the structure of interfaces influences the mobility and concentration of carriers that are responsible for transport. Using low angle twist grain boundaries in MgO as a model system, we examine the structural and kinetic properties of vacancies. These boundaries are characterized by a network of screw dislocations. Vacancies of both types, Mg and O, are strongly attracted to the dislocation network, residing preferentially at the misfit dislocation intersections (MDIs). However, the vacancies can lower their energy by splitting into two parts, which then repel each other along the dislocation line between two MDIs, further lowering their energy. This dissociated structure has important consequences for transport, as the free energy of the dissociated vacancies decreases with decreasing twist angle, leading to an increase in the net migration barrier for diffusion as revealed by molecular dynamics simulations. Similar behavior is observed in BaO and NaCl, highlighting the generality of the behavior. Finally, we analyze the structure of the dissociated vacancies as a pair of jogs on the dislocation and construct a model containing electrostatic and elastic contributions that qualitatively describe the energetics of the dissociated vacancy. Our results represent the first validation of a mechanism for vacancy dissociation on screw dislocations in ionic materials first discussed by Thomson and Balluffi in 1962.

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Research Organization:: Los Alamos National Laboratory (LANL)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1438122

Report Number(s):: LA-UR-18-20967

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 6 Vol. 30; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (51)

Interatomic potential models for natural apatite crystals: Incorporating strontium and the lanthanides Rabone, J. A. L.; De Leeuw, N. H. Journal of Computational Chemistry, Vol. 27, Issue 2 https://doi.org/10.1002/jcc.20323	journal	January 2005
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
Dislocation theory Frank, F. C. Il Nuovo Cimento, Vol. 7, Issue S2 https://doi.org/10.1007/BF02751488	journal	September 1958
Molecular dynamics of ionic self-diffusion at an MgO grain boundary Landuzzi, Fabio; Pasquini, Luca; Giusepponi, Simone Journal of Materials Science, Vol. 50, Issue 6 https://doi.org/10.1007/s10853-014-8808-9	journal	January 2015
Molecular dynamics study of the threshold displacement energy in MgO Park, Byeongwon; Weber, William J.; Corrales, L. René Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 166-167 https://doi.org/10.1016/S0168-583X(99)00694-1	journal	May 2000
The relative free energies of grain boundaries in magnesia as a function of five macroscopic parameters Saylor, David M.; Morawiec, Adam; Rohrer, Gregory S. Acta Materialia, Vol. 51, Issue 13 https://doi.org/10.1016/S1359-6454(03)00182-4	journal	August 2003
Uranium vacancy mobility at the Σ5 symmetric tilt and Σ5 twist grain boundaries in UO2 Uberuaga, Blas Pedro; Andersson, David A. Computational Materials Science, Vol. 108 https://doi.org/10.1016/j.commatsci.2015.06.017	journal	October 2015
Ab initio molecular dynamics simulations of low energy recoil events in MgO Petersen, B. A.; Liu, B.; Weber, W. J. Journal of Nuclear Materials, Vol. 486 https://doi.org/10.1016/j.jnucmat.2017.01.020	journal	April 2017
Simulations of cascades in pure and alumina doped magnesia Cleave, Antony R.; Grimes, Robin W.; Smith, Roger Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 250, Issue 1-2 https://doi.org/10.1016/j.nimb.2006.04.080	journal	September 2006
Grain boundary character dependence of oxygen grain boundary diffusion in α-Al2O3 bicrystals Nakagawa, Tsubasa; Nishimura, Hitoshi; Sakaguchi, Isao Scripta Materialia, Vol. 65, Issue 6 https://doi.org/10.1016/j.scriptamat.2011.06.024	journal	September 2011
Dislocations Accelerate Oxygen Ion Diffusion in La _0.8 Sr _0.2 MnO ₃ Epitaxial Thin Films Navickas, Edvinas; Chen, Yan; Lu, Qiyang ACS Nano, Vol. 11, Issue 11 https://doi.org/10.1021/acsnano.7b06228	journal	September 2017
Electronic and Chemical Properties of a Surface-Terminated Screw Dislocation in MgO McKenna, Keith P. Journal of the American Chemical Society, Vol. 135, Issue 50 https://doi.org/10.1021/ja408342z	journal	December 2013
Dislocations in SrTiO ₃ : Easy To Reduce but Not so Fast for Oxygen Transport Marrocchelli, Dario; Sun, Lixin; Yildiz, Bilge Journal of the American Chemical Society, Vol. 137, Issue 14 https://doi.org/10.1021/ja513176u	journal	April 2015
Nonrandom Point Defect Configurations and Driving Force Transitions for Grain Boundary Segregation in Trivalent Cation Doped ZrO ₂ Yokoi, T.; Yoshiya, M.; Yasuda, H. Langmuir, Vol. 30, Issue 47 https://doi.org/10.1021/la503338x	journal	November 2014
Atomistic Modeling of Point Defects and Diffusion in Copper Grain Boundaries Suzuki, A.; Mishin, Y. Interface Science, Vol. 11, Issue 1, p. 131-148 https://doi.org/10.1023/A:1021599310093	journal	January 2003
Termination chemistry-driven dislocation structure at SrTiO3/MgO heterointerfaces Dholabhai, Pratik P.; Pilania, Ghanshyam; Aguiar, Jeffery A. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6043	journal	September 2014
Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects Sun, Lixin; Marrocchelli, Dario; Yildiz, Bilge Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7294	journal	February 2015
The relationship between grain boundary structure, defect mobility and grain boundary sink efficiency Uberuaga, Blas Pedro; Vernon, Louis J.; Martinez, Enrique Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep09095	journal	March 2015
Do dislocations act as atomic autobahns for oxygen in the perovskite oxide SrTiO ₃ ? Metlenko, Veronika; Ramadan, Amr H. H.; Gunkel, Felix Nanoscale, Vol. 6, Issue 21 https://doi.org/10.1039/C4NR04083J	journal	January 2014
On the mobility of carriers at semi-coherent oxide heterointerfaces Dholabhai, Pratik P.; Martínez, Enrique; Brown, Nicholas T. Physical Chemistry Chemical Physics, Vol. 19, Issue 34 https://doi.org/10.1039/C7CP04884J	journal	January 2017
Defects and dislocations in MgO: atomic scale models of impurity segregation and fast pipe diffusion Zhang, Feiwu; Walker, Andrew M.; Wright, Kate Journal of Materials Chemistry, Vol. 20, Issue 46 https://doi.org/10.1039/c0jm01550d	journal	January 2010
Dislocation-enhanced ionic conductivity of yttria-stabilized zirconia Otsuka, Kazuya; Kuwabara, Akihide; Nakamura, Atsutomo Applied Physics Letters, Vol. 82, Issue 6 https://doi.org/10.1063/1.1544440	journal	February 2003
Kinetic Theory of Dislocation Climb. I. General Models for Edge and Screw Dislocations Thomson, R. M.; Balluffi, R. W. Journal of Applied Physics, Vol. 33, Issue 3 https://doi.org/10.1063/1.1777171	journal	March 1962
Charged dislocations in ionic crystals Whitworth, R. W. Advances in Physics, Vol. 24, Issue 2 https://doi.org/10.1080/00018737500101401	journal	March 1975
Secondary grain boundary dislocations in [001] twist boundaries in MgO I. Intrinsic structures Sun, C. P.; Balluffi, R. W. Philosophical Magazine A, Vol. 46, Issue 1 https://doi.org/10.1080/01418618208236206	journal	July 1982
On the structure of twist grain boundaries in ionic oxides Tasker, P. W.; Duffy, D. M. Philosophical Magazine A, Vol. 47, Issue 6 https://doi.org/10.1080/01418618308243118	journal	June 1983
Atomistic simulation of the effect of temperature and pressure on the [001] symmetric tilt grain boundaries of MgO Harris, D. J.; Watson, G. W.; Parker, S. C. Philosophical Magazine A, Vol. 74, Issue 2 https://doi.org/10.1080/01418619608242151	journal	August 1996
The General Utility Lattice Program ( GULP ) Gale, Julian D.; Rohl, Andrew L. Molecular Simulation, Vol. 29, Issue 5 https://doi.org/10.1080/0892702031000104887	journal	May 2003
Atomistic simulation of oxide dislocations and interfaces Parker, S. C.; De Leeuw, N. H.; Harris, D. J. Radiation Effects and Defects in Solids, Vol. 151, Issue 1-4 https://doi.org/10.1080/10420159908245954	journal	November 1999
Potential models for ionic oxides Lewis, G. V.; Catlow, C. R. A. Journal of Physics C: Solid State Physics, Vol. 18, Issue 6 https://doi.org/10.1088/0022-3719/18/6/010	journal	February 1985
Point defect–grain boundary interactions in MgO: an atomistic study Uberuaga, Blas Pedro; Bai, Xian-Ming; Dholabhai, Pratik P. Journal of Physics: Condensed Matter, Vol. 25, Issue 35 https://doi.org/10.1088/0953-8984/25/35/355001	journal	July 2013
AtomEye: an efficient atomistic configuration viewer Li, Ju Modelling and Simulation in Materials Science and Engineering, Vol. 11, Issue 2 https://doi.org/10.1088/0965-0393/11/2/305	journal	January 2003
Peierls–Nabarro modelling of dislocations in MgO from ambient pressure to 100 GPa Carrez, Philippe; Ferré, Denise; Cordier, Patrick Modelling and Simulation in Materials Science and Engineering, Vol. 17, Issue 3 https://doi.org/10.1088/0965-0393/17/3/035010	journal	February 2009
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
Extracting dislocations and non-dislocation crystal defects from atomistic simulation data Stukowski, Alexander; Albe, Karsten Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 8 https://doi.org/10.1088/0965-0393/18/8/085001	journal	September 2010
Vacancies at the Cu–Nb semicoherent interface Metsanurk, E.; Tamm, A.; Aabloo, A. Modelling and Simulation in Materials Science and Engineering, Vol. 25, Issue 2 https://doi.org/10.1088/1361-651X/25/2/025012	journal	January 2017
Vacancy migration at the {410}/[001] symmetric tilt grain boundary of MgO: An atomistic simulation study Harris, D. J.; Watson, G. W.; Parker, S. C. Physical Review B, Vol. 56, Issue 18 https://doi.org/10.1103/PhysRevB.56.11477	journal	November 1997
Computer simulation of general grain boundaries in rocksalt oxides Harding, J. H.; Harris, D. J.; Parker, S. C. Physical Review B, Vol. 60, Issue 4 https://doi.org/10.1103/PhysRevB.60.2740	journal	July 1999
Diffusion mechanisms in Cu grain boundaries Sørensen, Mads R.; Mishin, Yuri; Voter, Arthur F. Physical Review B, Vol. 62, Issue 6 https://doi.org/10.1103/PhysRevB.62.3658	journal	August 2000
Dynamical simulations of radiation damage and defect mobility in MgO Uberuaga, B. P.; Smith, R.; Cleave, A. R. Physical Review B, Vol. 71, Issue 10 https://doi.org/10.1103/PhysRevB.71.104102	journal	March 2005
First-principles calculations of defects near a grain boundary in MgO McKenna, K. P.; Shluger, A. L. Physical Review B, Vol. 79, Issue 22 https://doi.org/10.1103/PhysRevB.79.224116	journal	June 2009
Dislocation mechanism of interface point defect migration Kolluri, Kedarnath; Demkowicz, Michael J. Physical Review B, Vol. 82, Issue 19 https://doi.org/10.1103/PhysRevB.82.193404	journal	November 2010
Structure of a 2 ∘ (010) Cu twist boundary interface and the segregation of vacancies and He atoms Martínez, Enrique; Hirth, John P.; Nastasi, Michael Physical Review B, Vol. 85, Issue 6 https://doi.org/10.1103/PhysRevB.85.060101	journal	February 2012
Formation, migration, and clustering of delocalized vacancies and interstitials at a solid-state semicoherent interface Kolluri, Kedarnath; Demkowicz, Michael J. Physical Review B, Vol. 85, Issue 20 https://doi.org/10.1103/PhysRevB.85.205416	journal	May 2012
Atomistic modeling of long-term evolution of twist boundaries under vacancy supersaturation Martínez, Enrique; Caro, Alfredo Physical Review B, Vol. 86, Issue 21 https://doi.org/10.1103/PhysRevB.86.214109	journal	December 2012
Interface Structure and Radiation Damage Resistance in Cu-Nb Multilayer Nanocomposites Demkowicz, M. J.; Hoagland, R. G.; Hirth, J. P. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136102	journal	April 2008
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
Observation of Giant Diffusivity Along Dislocation Cores Legros, M.; Dehm, G.; Arzt, E. Science, Vol. 319, Issue 5870 https://doi.org/10.1126/science.1151771	journal	March 2008
Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures Garcia-Barriocanal, J.; Rivera-Calzada, A.; Varela, M. Science, Vol. 321, Issue 5889 https://doi.org/10.1126/science.1156393	journal	August 2008
Nudged elastic band method for finding minimum energy paths of transitions JÓNsson, Hannes; Mills, Greg; Jacobsen, Karsten W. Proceedings of the International School of Physics, Classical and Quantum Dynamics in Condensed Phase Simulations https://doi.org/10.1142/9789812839664_0016	conference	November 2011
Interstitial diffusion along twist grain boundaries in Cu Nomura, Miki; Adams, James B. Journal of Materials Research, Vol. 10, Issue 11 https://doi.org/10.1557/JMR.1995.2916	journal	November 1995

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