Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides
The Ruddlesden–Popper (RP) layered perovskite structure is of great interest due to its inherent tunability, and the emergence and growth of the compositionally complex oxide (CCO) concept endows the RP family with further possibilities. Here, a comprehensive assessment of thermodynamic stabilizatio...
| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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AIP Publishing LLC
2023-05-01
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| Series: | APL Materials |
| Online Access: | http://dx.doi.org/10.1063/5.0144766 |
| _version_ | 1797771775086428160 |
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| author | Bo Jiang Krishna Chaitanya Pitike De-Ye Lin Stephen C. Purdy Xin Wang Yafan Zhao Yuanpeng Zhang Peter Metz Antonio Macias Harry M. Meyer III Albina Y. Borisevich Jiaqiang Yan Valentino R. Cooper Craig A. Bridges Katharine Page |
| author_facet | Bo Jiang Krishna Chaitanya Pitike De-Ye Lin Stephen C. Purdy Xin Wang Yafan Zhao Yuanpeng Zhang Peter Metz Antonio Macias Harry M. Meyer III Albina Y. Borisevich Jiaqiang Yan Valentino R. Cooper Craig A. Bridges Katharine Page |
| author_sort | Bo Jiang |
| collection | DOAJ |
| description | The Ruddlesden–Popper (RP) layered perovskite structure is of great interest due to its inherent tunability, and the emergence and growth of the compositionally complex oxide (CCO) concept endows the RP family with further possibilities. Here, a comprehensive assessment of thermodynamic stabilization, local order/disorder, and lattice distortion was performed in the first two reported examples of lanthanum-deficient Lan+1BnO3n+1 (n = 1, B = Mg, Co, Ni, Cu, Zn) obtained via various processing conditions. Chemical short-range order (CSRO) at the B-site and the controllable excess interstitial oxygen (δ) in RP-CCOs are uncovered by neutron pair distribution function analysis. Reverse Monte Carlo analysis of the data, Metropolis Monte Carlo simulations, and extended x-ray absorption fine structure analysis implies a modest degree of magnetic element segregation on the local scale. Further, ab initio molecular dynamics simulations results obtained from special quasirandom structure disagree with experimentally observed CSRO but confirm Jahn–Teller distortion of CuO6 octahedra. These findings highlight potential opportunities to control local order/disorder and excess interstitial oxygen in layered RP-CCOs and demonstrate a high degree of freedom for tailoring application-specific properties. They also suggest a need for expansion of theoretical and data modeling approaches in order to meet the innate challenges of CCO and related high-entropy phases. |
| first_indexed | 2024-03-12T21:42:33Z |
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| id | doaj.art-979c8f85d4664cd28f39edd3f09651e3 |
| institution | Directory Open Access Journal |
| issn | 2166-532X |
| language | English |
| last_indexed | 2024-03-12T21:42:33Z |
| publishDate | 2023-05-01 |
| publisher | AIP Publishing LLC |
| record_format | Article |
| series | APL Materials |
| spelling | doaj.art-979c8f85d4664cd28f39edd3f09651e32023-07-26T15:44:37ZengAIP Publishing LLCAPL Materials2166-532X2023-05-01115051104051104-1310.1063/5.0144766Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxidesBo Jiang0Krishna Chaitanya Pitike1De-Ye Lin2Stephen C. Purdy3Xin Wang4Yafan Zhao5Yuanpeng Zhang6Peter Metz7Antonio Macias8Harry M. Meyer III9Albina Y. Borisevich10Jiaqiang Yan11Valentino R. Cooper12Craig A. Bridges13Katharine Page14Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAMaterials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAInstitute of Applied Physics and Computational Mathematics, Huayuan Road 6, Beijing 100088, China and CAEP Software Center for High Performance Numercial Simulation, Huayuan Road 6, Beijing 100088, ChinaNeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USADepartment of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, USAInstitute of Applied Physics and Computational Mathematics, Huayuan Road 6, Beijing 100088, China and CAEP Software Center for High Performance Numercial Simulation, Huayuan Road 6, Beijing 100088, ChinaNeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USADepartment of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, USANeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAMaterials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USACenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAMaterials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAMaterials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAChemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USANeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USAThe Ruddlesden–Popper (RP) layered perovskite structure is of great interest due to its inherent tunability, and the emergence and growth of the compositionally complex oxide (CCO) concept endows the RP family with further possibilities. Here, a comprehensive assessment of thermodynamic stabilization, local order/disorder, and lattice distortion was performed in the first two reported examples of lanthanum-deficient Lan+1BnO3n+1 (n = 1, B = Mg, Co, Ni, Cu, Zn) obtained via various processing conditions. Chemical short-range order (CSRO) at the B-site and the controllable excess interstitial oxygen (δ) in RP-CCOs are uncovered by neutron pair distribution function analysis. Reverse Monte Carlo analysis of the data, Metropolis Monte Carlo simulations, and extended x-ray absorption fine structure analysis implies a modest degree of magnetic element segregation on the local scale. Further, ab initio molecular dynamics simulations results obtained from special quasirandom structure disagree with experimentally observed CSRO but confirm Jahn–Teller distortion of CuO6 octahedra. These findings highlight potential opportunities to control local order/disorder and excess interstitial oxygen in layered RP-CCOs and demonstrate a high degree of freedom for tailoring application-specific properties. They also suggest a need for expansion of theoretical and data modeling approaches in order to meet the innate challenges of CCO and related high-entropy phases.http://dx.doi.org/10.1063/5.0144766 |
| spellingShingle | Bo Jiang Krishna Chaitanya Pitike De-Ye Lin Stephen C. Purdy Xin Wang Yafan Zhao Yuanpeng Zhang Peter Metz Antonio Macias Harry M. Meyer III Albina Y. Borisevich Jiaqiang Yan Valentino R. Cooper Craig A. Bridges Katharine Page Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides APL Materials |
| title | Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides |
| title_full | Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides |
| title_fullStr | Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides |
| title_full_unstemmed | Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides |
| title_short | Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides |
| title_sort | local cation ordering in compositionally complex ruddlesden popper n 1 oxides |
| url | http://dx.doi.org/10.1063/5.0144766 |
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