Anti-phase boundary accelerated exsolution of nanoparticles in non-stoichiometric perovskite thin films

Hyeon Han (), Yaolong Xing, Bumsu Park, Dmitry I. Bazhanov, Yeongrok Jin, John T. S. Irvine, Jaekwang Lee and Sang Ho Oh ()
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Hyeon Han: Max Planck Institute of Microstructure Physics, Weinberg 2
Yaolong Xing: Sungkyunkwan University
Bumsu Park: Sungkyunkwan University
Dmitry I. Bazhanov: Moscow State University, GSP-1, Leninskye Gory,1-2
Yeongrok Jin: Pusan National University
John T. S. Irvine: University of St Andrews
Jaekwang Lee: Pusan National University
Sang Ho Oh: Sungkyunkwan University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Exsolution of excess transition metal cations from a non-stoichiometric perovskite oxide has sparked interest as a facile route for the formation of stable nanoparticles on the oxide surface. However, the atomic-scale mechanism of this nanoparticle formation remains largely unknown. The present in situ scanning transmission electron microscopy combined with density functional theory calculation revealed that the anti-phase boundaries (APBs) characterized by the a/2 type lattice displacement accommodate the excess B-site cation (Ni) through the edge-sharing of BO6 octahedra in a non-stoichiometric ABO3 perovskite oxide (La0.2Sr0.7Ni0.1Ti0.9O3-δ) and provide the fast diffusion pathways for nanoparticle formation by exsolution. Moreover, the APBs further promote the outward diffusion of the excess Ni toward the surface as the segregation energy of Ni is lower at the APB/surface intersection. The formation of nanoparticles occurs through the two-step crystallization mechanism, i.e., the nucleation of an amorphous phase followed by crystallization, and via reactive wetting on the oxide support, which facilitates the formation of a stable triple junction and coherent interface, leading to the distinct socketing of nanoparticles to the oxide support. The atomic-scale mechanism unveiled in this study can provide insights into the design of highly stable nanostructures.

Date: 2022
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DOI: 10.1038/s41467-022-34289-3

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