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Title: Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics

Abstract

We report on the selective fabrication of high-quality Sr 2IrO 4 and SrIrO 3 epitaxial thin films from a single polycrystalline Sr2IrO4 target by pulsed laser deposition. Using a combination of x-ray diffraction and photoemission spectroscopy characterizations, we discover that within a relatively narrow range of substrate temperature, the oxygen partial pressure plays a critical role in the cation stoichiometric ratio of the films, and triggers the stabilization of different Ruddlesden-Popper (RP) phases. Resonant x-ray absorption spectroscopy measurements taken at the Ir L edge and the O K edge demonstrate the presence of strong spin-orbit coupling, and reveal the electronic and orbital structures of both compounds. These results suggest that in addition to the conventional thermodynamics consideration, higher members of the Sr n+1Ir nO 3n+1 series can possibly be achieved by kinetic control away from the thermodynamic limit. These findings offer an approach to the synthesis of ultrathin films of the RP series of iridates and can be extended to other complex oxides with layered structure.

Authors:
 [1];  [2];  [1];  [3];  [1];  [4];  [5];  [4];  [5];  [1]
  1. Rutgers Univ., Piscataway, NJ (United States). Dept. of Physics and Astronomy
  2. Rutgers Univ., Piscataway, NJ (United States). Dept. of Physics and Astronomy; Chinese Academy of Sciences (CAS), Zhejiang (China). Ningbo Inst. of Materials Technology and Engineering
  3. Indian Inst. of Science, Bengaluru (India). Dept. of Physics
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); Gordon and Betty Moore Foundation
OSTI Identifier:
1422577
Alternate Identifier(s):
OSTI ID: 1414625
Grant/Contract Number:  
AC02-06CH11357; SC0012375; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 7; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Liu, Xiaoran, Cao, Yanwei, Pal, B., Middey, S., Kareev, M., Choi, Y., Shafer, P., Haskel, D., Arenholz, E., and Chakhalian, J. Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics. United States: N. p., 2017. Web. doi:10.1103/PhysRevMaterials.1.075004.
Liu, Xiaoran, Cao, Yanwei, Pal, B., Middey, S., Kareev, M., Choi, Y., Shafer, P., Haskel, D., Arenholz, E., & Chakhalian, J. Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics. United States. doi:10.1103/PhysRevMaterials.1.075004.
Liu, Xiaoran, Cao, Yanwei, Pal, B., Middey, S., Kareev, M., Choi, Y., Shafer, P., Haskel, D., Arenholz, E., and Chakhalian, J. Fri . "Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics". United States. doi:10.1103/PhysRevMaterials.1.075004. https://www.osti.gov/servlets/purl/1422577.
@article{osti_1422577,
title = {Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics},
author = {Liu, Xiaoran and Cao, Yanwei and Pal, B. and Middey, S. and Kareev, M. and Choi, Y. and Shafer, P. and Haskel, D. and Arenholz, E. and Chakhalian, J.},
abstractNote = {We report on the selective fabrication of high-quality Sr2IrO4 and SrIrO3 epitaxial thin films from a single polycrystalline Sr2IrO4 target by pulsed laser deposition. Using a combination of x-ray diffraction and photoemission spectroscopy characterizations, we discover that within a relatively narrow range of substrate temperature, the oxygen partial pressure plays a critical role in the cation stoichiometric ratio of the films, and triggers the stabilization of different Ruddlesden-Popper (RP) phases. Resonant x-ray absorption spectroscopy measurements taken at the Ir L edge and the O K edge demonstrate the presence of strong spin-orbit coupling, and reveal the electronic and orbital structures of both compounds. These results suggest that in addition to the conventional thermodynamics consideration, higher members of the Srn+1IrnO3n+1 series can possibly be achieved by kinetic control away from the thermodynamic limit. These findings offer an approach to the synthesis of ultrathin films of the RP series of iridates and can be extended to other complex oxides with layered structure.},
doi = {10.1103/PhysRevMaterials.1.075004},
journal = {Physical Review Materials},
issn = {2475-9953},
number = 7,
volume = 1,
place = {United States},
year = {2017},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 3 works
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Figures / Tables:

Figure 1 Figure 1: Crystal structures of $Sr_{n+1}Ir_nO_{3n+1}$ Ruddlesden-Popper phases: $Sr_2IrO_4$ (n = 1), $Sr_{3}Ir_2O_7$ (n = 2), and $SrIrO_3$ (n = ∞).

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Works referenced in this record:

Enhanced oxygen reduction activity on surface-decorated perovskite thin films for solid oxide fuel cells
journal, January 2011

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Cobalt Assisted Synthesis of IrCu Hollow Octahedral Nanocages as Highly Active Electrocatalysts toward Oxygen Evolution Reaction
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Engineering 1D Quantum Stripes from Superlattices of 2D Layered Materials
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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.