Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction
Abstract Double perovskite oxides, with generalized formula A2BB $$^{\prime}$$ ′ O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limita...
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Nature Portfolio
2021
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oai:doaj.org-article:72d209f7cfe74227b6345e0efb5cdd0b2021-12-02T17:40:01ZStudy of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction10.1038/s41524-021-00561-12057-3960https://doaj.org/article/72d209f7cfe74227b6345e0efb5cdd0b2021-06-01T00:00:00Zhttps://doi.org/10.1038/s41524-021-00561-1https://doaj.org/toc/2057-3960Abstract Double perovskite oxides, with generalized formula A2BB $$^{\prime}$$ ′ O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La2TiFeO6 and La2VCuO6 films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La2TiFeO6, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides.Edoardo FertittaSujit DasDebalina BanerjeeFarbod EbrahimiClément BarraudKai DuHe TianChris J. PickardCedric WeberRamamoorthy RameshPeter LittlewoodDavid DubbinkNature PortfolioarticleMaterials of engineering and construction. Mechanics of materialsTA401-492Computer softwareQA76.75-76.765ENnpj Computational Materials, Vol 7, Iss 1, Pp 1-8 (2021) |
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Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765 |
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Materials of engineering and construction. Mechanics of materials TA401-492 Computer software QA76.75-76.765 Edoardo Fertitta Sujit Das Debalina Banerjee Farbod Ebrahimi Clément Barraud Kai Du He Tian Chris J. Pickard Cedric Weber Ramamoorthy Ramesh Peter Littlewood David Dubbink Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| description |
Abstract Double perovskite oxides, with generalized formula A2BB $$^{\prime}$$ ′ O6, attract wide interest due to their multiferroic and charge transfer properties. They offer a wide range of potential applications such as spintronics and electrically tunable devices. However, great practical limitations are encountered, since a spontaneous order of the B-site cations is notoriously hard to achieve. In this joint experimental-theoretical work, we focused on the characterization of double perovskites La2TiFeO6 and La2VCuO6 films grown by pulsed laser deposition and interpretation of the observed B-site disorder and partial charge transfer between the B-site ions. A random structure sampling method was used to show that several phases compete due to their corresponding configurational entropy. In order to capture a representative picture of the most relevant competing microstates in realistic experimental conditions, this search included the potential formation of non-stoichiometric phases as well, which could also be directly related to the observed partial charge transfer. We optimized the information encapsulated in the potential energy landscape, captured via structure sampling, by evaluating both enthalpic and entropic terms. These terms were employed as a metric for the competition of different phases. This approach, applied herein specifically to La2TiFeO6, highlights the presence of highly entropic phases above the ground state which can explain the disorder observed frequently in the broader class of double perovskite oxides. |
| format |
article |
| author |
Edoardo Fertitta Sujit Das Debalina Banerjee Farbod Ebrahimi Clément Barraud Kai Du He Tian Chris J. Pickard Cedric Weber Ramamoorthy Ramesh Peter Littlewood David Dubbink |
| author_facet |
Edoardo Fertitta Sujit Das Debalina Banerjee Farbod Ebrahimi Clément Barraud Kai Du He Tian Chris J. Pickard Cedric Weber Ramamoorthy Ramesh Peter Littlewood David Dubbink |
| author_sort |
Edoardo Fertitta |
| title |
Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| title_short |
Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| title_full |
Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| title_fullStr |
Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| title_full_unstemmed |
Study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| title_sort |
study of disorder in pulsed laser deposited double perovskite oxides by first-principle structure prediction |
| publisher |
Nature Portfolio |
| publishDate |
2021 |
| url |
https://doaj.org/article/72d209f7cfe74227b6345e0efb5cdd0b |
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