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Abstract Grain-boundary (GB) structures are commonly imaged as discrete atomic columns, yet the chemical modifications are gradual and extend into the adjacent lattices, notably the space charge, hence the two-dimensional defects may also be treated as continuum changes to extended interfacial structure. This review presents a spatially-resolved analysis by electron energy-loss spectroscopy of the GB chemical structures in a series of SrTiO3 bicrystals and a ceramic, using analytical electron microscopy of the pre-Cs-correction era. It has identified and separated a transient layer at the model Σ5 grain-boundaries (GBs) with characteristic chemical bonding, extending the continuum interfacial approach to redefine the GB chemical structure. This GB layer has evolved under segregation of iron dopant, starting from subtle changes in local bonds until a clear transition into a distinctive GB chemistry with substantially increased titanium concentration confined within the GB layer in 3-unit cells, heavily strained, and with less strontium. Similar segregated GB layer turns into a titania-based amorphous film in SrTiO3 ceramic, hence reaching a more stable chemical structure in equilibrium with the intergranular Ti2O3 glass also. Space charge was not found by acceptor doping in both the strained Σ5 and amorphous GBs in SrTiO3 owing to the native transient nature of the GB layer that facilitates the transitions induced by Fe segregation into novel chemical structures subject to local and global equilibria. These GB transitions may add a new dimension into the structure-property relationship of the electronic materials.
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Received: 08 April 2018
Revised: 14 May 2018
Accepted manuscript online:
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PACS:
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05.70.Np
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(Interface and surface thermodynamics)
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68.35.Dv
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(Composition, segregation; defects and impurities)
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68.37.Ma
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(Scanning transmission electron microscopy (STEM))
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81.70.Jb
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(Chemical composition analysis, chemical depth and dopant profiling)
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Fund: Project supported by the National Natural Science Foundation of China (Grant No.51532006),the Fund from Shanghai Municipal Science and Technology Commission (Grant No.16DZ2260600),the 111 Project of the Ministry of Education,and the Fund from the National Bureau of Foreign Experts (Project No.D16002). |
Corresponding Authors:
Hui Gu
E-mail: gujiaoshou@shu.edu.cn
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Cite this article:
Hui Gu(顾辉) Chemical structure of grain-boundary layer in SrTiO3 and its segregation-induced transition: A continuum interface approach 2018 Chin. Phys. B 27 060503
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