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 · Mon Mar 05 00:00:00 EST 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), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1438122

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

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 3 works

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