4.8 Article

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

期刊

ACS NANO
卷 14, 期 10, 页码 13030-13037

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c04487

关键词

configurational complexity; cuprate; synthesis; high entropy oxides; phase transition; epitaxy

资金

  1. U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Materials Sciences and Engineering Division
  2. U.S. Department of Energy, Office of Science [DE-AC02-06CH11357]
  3. U.S. DOE Office of Science User Facilities at Brookhaven National Laboratory [DE-SC0012704]
  4. U.S. Department of Energy's National Nuclear Security Administration [DE-NA0003525]

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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 A(2)CuO(4) 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)(2)CuO4 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 similar to 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.

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