Applying Configurational Complexity to the 2D Ruddlesden–Popper Crystal Structure

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

doi:10.1021/acsnano.0c04487

Applying Configurational Complexity to the 2D Ruddlesden–Popper Crystal Structure

Journal Article · Tue Sep 15 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c04487· OSTI ID:1725852

Zhang, Wenrui ^[1]; Mazza, Alessandro R. ^[1]; Skoropata, Elizabeth ^[1]; ^[1]; ^[2]; Zhang, Jie ^[1]; Keppens, Veerle M. ^[2]; Zhang, Lihua ^[3]; Kisslinger, Kim ^[3]; Stavitski, Eli ^[3]; Brahlek, Matthew ^[1]; Freeland, John W. ^[4]; Lu, Ping ^[5]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

The layered Ruddlesden–Popper crystal structure can host a broad range of functionally important behaviors. In this work, 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 (La_0.2Pr_0.2Nd_0.2Sm_0.2Eu_0.2)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, energy-dispersive 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 Cu_X2O₄ 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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC04-94AL85000; SC0012704; NA0003525; AC05-00OR22725

OSTI ID:: 1725852

Alternate ID(s):: OSTI ID: 1813053
OSTI ID: 1761621
OSTI ID: 1763318

Report Number(s):: SAND--2020-12941J; 692387

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 10 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
configurational complexity
cuprate
epitaxy
high entropy oxides
phase transition
synthesis

Applying Configurational Complexity to the 2D Ruddlesden–Popper Crystal Structure

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