Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides

Jiang, Bo; Pitike, Krishna Chaitanya; Lin, De-Ye; Purdy, Stephen C.; Wang, Xin; Zhao, Yafan; Zhang, Yuanpeng; Metz, Peter; Macias, Antonio; Meyer, III, Harry M.; Borisevich, Albina Y.; Yan, Jiaqiang; Cooper, Valentino R.; Bridges, Craig A.; Page, Katharine

doi:10.1063/5.0144766

Title: Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides

Journal Article · Tue May 02 00:00:00 EDT 2023 · APL Materials

DOI:https://doi.org/10.1063/5.0144766· OSTI ID:1999042

Jiang, Bo ^[1];

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Institute of Applied Physics and Computational Mathematics, Beijing (China); CAEP Software Center for High Performance Numerical Simulation, Beijing (China)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, Los Angeles, CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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 La_n+1B_nO_3n+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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1999042

Journal Information:: APL Materials, Vol. 11, Issue 5; ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
Ruddlesden-Popper
local structure
interstitial oxygen
neutron total scattering
DFT
EX-AFS

Title: Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides

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