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Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure

Sachan, Ritesh and Cooper, Valentino R. and Liu, Bin and Aidhy, Dilpuneet S. and Voas, Brian K. and Lang, Maik and Ou, Xin and Trautmann, Christina and Zhang, Yanwen and Chisholm, Matthew F. and Weber, William J. (2017):
Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure.
In: The Journal of Physical Chemistry C, American Chemical Society Publications, pp. 975-981, 121, (1), ISSN 1932-7447, DOI: 10.1021/acs.jpcc.6b12522, [Online-Edition: https://doi.org/10.1021/acs.jpcc.6b12522],
[Article]

Abstract

Atomically disordered oxides have attracted significant attention in recent years due to the possibility of enhanced ionic conductivity. However, the correlation between atomic disorder, corresponding electronic structure, and the resulting oxygen diffusivity is not well understood. The disordered variants of the ordered pyrochlore structure in gadolinium titanate (Gd2Ti2O7) are seen as a particularly interesting prospect due to intrinsic presence of a vacant oxygen site in the unit atomic structure, which could provide a channel for fast oxygen conduction. In the present work, we provide insights into the subangstrom scale on the disordering-induced variations in the local atomic environment and its effect on the electronic structure in high-energy ion irradiation-induced disordered nanochannels, which can be utilized as pathways for fast oxygen ion transport. With the help of an atomic plane-by-plane-resolved analyses, the work shows how the presence of various types of TiOx polyhedral that exist in the amorphous and disordered crystalline phase modify the electronic structures relative to the ordered pyrochlore phase in Gd2Ti2O7. The correlated molecular dynamics simulations on the disordered structures show a remarkable enhancement in oxygen diffusivity as compared with ordered pyrochlore lattice and make that a suitable candidate for applications requiring fast oxygen conduction.

Item Type: Article
Erschienen: 2017
Creators: Sachan, Ritesh and Cooper, Valentino R. and Liu, Bin and Aidhy, Dilpuneet S. and Voas, Brian K. and Lang, Maik and Ou, Xin and Trautmann, Christina and Zhang, Yanwen and Chisholm, Matthew F. and Weber, William J.
Title: Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure
Language: English
Abstract:

Atomically disordered oxides have attracted significant attention in recent years due to the possibility of enhanced ionic conductivity. However, the correlation between atomic disorder, corresponding electronic structure, and the resulting oxygen diffusivity is not well understood. The disordered variants of the ordered pyrochlore structure in gadolinium titanate (Gd2Ti2O7) are seen as a particularly interesting prospect due to intrinsic presence of a vacant oxygen site in the unit atomic structure, which could provide a channel for fast oxygen conduction. In the present work, we provide insights into the subangstrom scale on the disordering-induced variations in the local atomic environment and its effect on the electronic structure in high-energy ion irradiation-induced disordered nanochannels, which can be utilized as pathways for fast oxygen ion transport. With the help of an atomic plane-by-plane-resolved analyses, the work shows how the presence of various types of TiOx polyhedral that exist in the amorphous and disordered crystalline phase modify the electronic structures relative to the ordered pyrochlore phase in Gd2Ti2O7. The correlated molecular dynamics simulations on the disordered structures show a remarkable enhancement in oxygen diffusivity as compared with ordered pyrochlore lattice and make that a suitable candidate for applications requiring fast oxygen conduction.

Journal or Publication Title: The Journal of Physical Chemistry C
Volume: 121
Number: 1
Publisher: American Chemical Society Publications
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Ion-Beam-Modified Materials
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 29 Dec 2017 11:53
DOI: 10.1021/acs.jpcc.6b12522
Official URL: https://doi.org/10.1021/acs.jpcc.6b12522
Funders: This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division., V.R.C. was sponsored by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division through the Office of Science Early Career Research Program., B.K.V. acknowledges summer support through the HERE program at ORNL., M.L.’s contribution was supported as part of the Materials Science of Actinides, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0001089., This simulation used resources of the National Energy Research Scientific Computing Center, supported by the Office of Science, U.S. Department of Energy, under Contract No. DEAC02-05CH11231.
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