Applying configurational complexity to the 2d ruddlesden-popper crystal structure

Thomas Z. Ward, Wenrui Zhang, Alessandro R. Mazza, Elizabeth Skoropata, Debangshu Mukherjee, Brianna Musico, Jie Zhang, Veerle M. Keppens, Lihua Zhang, Kim Kisslinger, Eli Stavitski, Matthew Brahlek, John W. Freeland, Ping Lu

Research output: Contribution to journalArticlepeer-review

29 Scopus citations

Abstract

The layered Ruddlesden-Popper crystal structure can host a broad range of functionally important behaviors. Here we establish extraordinary configurational disorder in a layered Ruddlesden-Popper (RP) structure using entropy stabilization assisted synthesis. A protype A2CuO4 RP cuprate oxide with five cations on the A-site sublattice is designed and fabricated into epitaxial single crystal films using pulsed laser deposition. When grown on a near lattice matched substrate, the (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4 film features a T'-type RP structure with uniform A-site cation mixing and square-planar CuO4 units. These observations are made with a range of combined characterizations using X-ray diffraction, atomic-resolution scanning transmission electron microscopy, energydispersive X-ray spectroscopy, and X-ray absorption spectroscopy measurements. It is further found that heteroepitaxial strain plays an important role in crystal phase formation during synthesis. Compressive strain over ∼1.5% results in the formation of a non-RP cubic phase consistent with a CuX2O4 spinel structure. The ability to manipulate configurational complexity and move between 2D layered RP and 3D cubic crystal structures in cuprate and related materials promises to enable flexible design strategies for a range of functionalities, such as magnetoresistance, unconventional superconductivity, ferroelectricity, catalysis, and ion transport.

Original languageEnglish
Pages (from-to)13030-13037
Number of pages8
JournalACS Nano
Volume14
Issue number10
DOIs
StatePublished - Oct 27 2020

Funding

Experiment design, sample synthesis, and structural characterization were supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Part of the STEM characterization was conducted through user proposal at the Center for Nanophase Materials Sciences, which is a U.S. DOE, Office of Science User Facility. Soft X-ray spectroscopy at beamline 4-ID-C of the Advanced Photon Source, Argonne National Laboratory, was supported by the U.S. Department of Energy, Office of Science under Grant No. DE-AC02-06CH11357. This research used resources of the Center for Functional Nanomaterials and the Inner Shell Spectroscopy 8-ID beamline of the National Synchrotron Light Source II, which are U.S. DOE Office of Science User Facilities at Brookhaven National Laboratory under Contract No. DE-SC0012704. Sandia National Laboratories is a multiprogram laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government.

Keywords

  • Configurational complexity
  • Cuprate
  • Epitaxy
  • High entropy oxides
  • Phase transition
  • Synthesis

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