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Title: Epitaxial thin films of pyrochlore iridate Bi2+xIr2-yO7-δ: structure, defects and transport properties

Abstract

While pyrochlore iridate thin films are theoretically predicted to possess a variety of emergent topological properties, experimental verification of these predictions can be obstructed by the challenge in thin film growth. We report on the pulsed laser deposition and characterization of thin films of a representative pyrochlore compound Bi2Ir2O7. Moreover, the films were epitaxially grown on yttria-stabilized zirconia substrates and have lattice constants that are a few percent larger than that of the bulk single crystals. The film composition shows a strong dependence on the oxygen partial pressure. Density-functional-theory calculations indicate the existence of BiIr antisite defects, qualitatively consistent with the high Bi: Ir ratio found in the films. Both Ir and Bi have oxidation states that are lower than their nominal values, suggesting the existence of oxygen deficiency. The iridate thin films show a variety of intriguing transport characteristics, including multiple charge carriers, logarithmic dependence of resistance on temperature, antilocalization corrections to conductance due to spin-orbit interactions, and linear positive magnetoresistance.

Authors:
 [1];  [2];  [1];  [2]; ORCiD logo [3];  [4];  [5];  [1];  [1];  [1];  [2];  [3]; ORCiD logo [6];  [2];  [1]
  1. Indiana Univ., Bloomington, IN (United States). Dept. of Physics
  2. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Physics
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
  4. Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
  5. Indiana Univ., Bloomington, IN (United States). Dept. of Physics; Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
  6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies; State Univ. of New York (SUNY), Buffalo, NY (United States). Dept. of Materials Design and Innovation
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1396132
Report Number(s):
LA-UR-17-24496
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
AC52-06NA2539
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; surfaces, interfaces and thin films

Citation Formats

Yang, W. C., Xie, Y. T., Zhu, W. K., Park, K., Chen, A. P., Losovyj, Y., Li, Z., Liu, H. M., Starr, M., Acosta, J. A., Tao, C. G., Li, N., Jia, Q. X., Heremans, J. J., and Zhang, S. X. Epitaxial thin films of pyrochlore iridate Bi2+xIr2-yO7-δ: structure, defects and transport properties. United States: N. p., 2017. Web. doi:10.1038/s41598-017-06785-w.
Yang, W. C., Xie, Y. T., Zhu, W. K., Park, K., Chen, A. P., Losovyj, Y., Li, Z., Liu, H. M., Starr, M., Acosta, J. A., Tao, C. G., Li, N., Jia, Q. X., Heremans, J. J., & Zhang, S. X. Epitaxial thin films of pyrochlore iridate Bi2+xIr2-yO7-δ: structure, defects and transport properties. United States. https://doi.org/10.1038/s41598-017-06785-w
Yang, W. C., Xie, Y. T., Zhu, W. K., Park, K., Chen, A. P., Losovyj, Y., Li, Z., Liu, H. M., Starr, M., Acosta, J. A., Tao, C. G., Li, N., Jia, Q. X., Heremans, J. J., and Zhang, S. X. Thu . "Epitaxial thin films of pyrochlore iridate Bi2+xIr2-yO7-δ: structure, defects and transport properties". United States. https://doi.org/10.1038/s41598-017-06785-w. https://www.osti.gov/servlets/purl/1396132.
@article{osti_1396132,
title = {Epitaxial thin films of pyrochlore iridate Bi2+xIr2-yO7-δ: structure, defects and transport properties},
author = {Yang, W. C. and Xie, Y. T. and Zhu, W. K. and Park, K. and Chen, A. P. and Losovyj, Y. and Li, Z. and Liu, H. M. and Starr, M. and Acosta, J. A. and Tao, C. G. and Li, N. and Jia, Q. X. and Heremans, J. J. and Zhang, S. X.},
abstractNote = {While pyrochlore iridate thin films are theoretically predicted to possess a variety of emergent topological properties, experimental verification of these predictions can be obstructed by the challenge in thin film growth. We report on the pulsed laser deposition and characterization of thin films of a representative pyrochlore compound Bi2Ir2O7. Moreover, the films were epitaxially grown on yttria-stabilized zirconia substrates and have lattice constants that are a few percent larger than that of the bulk single crystals. The film composition shows a strong dependence on the oxygen partial pressure. Density-functional-theory calculations indicate the existence of BiIr antisite defects, qualitatively consistent with the high Bi: Ir ratio found in the films. Both Ir and Bi have oxidation states that are lower than their nominal values, suggesting the existence of oxygen deficiency. The iridate thin films show a variety of intriguing transport characteristics, including multiple charge carriers, logarithmic dependence of resistance on temperature, antilocalization corrections to conductance due to spin-orbit interactions, and linear positive magnetoresistance.},
doi = {10.1038/s41598-017-06785-w},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Thu Aug 10 00:00:00 EDT 2017},
month = {Thu Aug 10 00:00:00 EDT 2017}
}

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Works referenced in this record:

Topological Crystalline Insulators in Transition Metal Oxides
journal, April 2013


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Epitaxy-distorted spin-orbit Mott insulator in Sr 2 IrO 4 thin films
journal, February 2013


Suppression of metal-insulator transition at high pressure and pressure-induced magnetic ordering in pyrochlore oxide Nd 2 Ir 2 O 7
journal, January 2011


Emergence of Magnetic Long-range Order in Frustrated Pyrochlore Nd 2 Ir 2 O 7 with Metal–Insulator Transition
journal, March 2012

  • Tomiyasu, Keisuke; Matsuhira, Kazuyuki; Iwasa, Kazuaki
  • Journal of the Physical Society of Japan, Vol. 81, Issue 3
  • DOI: 10.1143/JPSJ.81.034709

Projector augmented-wave method
journal, December 1994


Metal-Nonmetal Changeover in Pyrochlore Iridates
journal, October 2001

  • Yanagishima, Daiki; Maeno, Yoshiteru
  • Journal of the Physical Society of Japan, Vol. 70, Issue 10
  • DOI: 10.1143/JPSJ.70.2880

Correlation effects in pyrochlore iridate thin films grown along the [111] direction
journal, August 2015


Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014


Mott physics and band topology in materials with strong spin–orbit interaction
journal, March 2010

  • Pesin, Dmytro; Balents, Leon
  • Nature Physics, Vol. 6, Issue 5
  • DOI: 10.1038/nphys1606

Odd-parity magnetoresistance in pyrochlore iridate thin films with broken time-reversal symmetry
journal, May 2015

  • Fujita, T. C.; Kozuka, Y.; Uchida, M.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09711

Similarities and Differences in the Structural and Electronic Properties of Ruthenium and Iridium PyrochloresA2M2O7−y(M=Ru, Ir)
journal, March 1998

  • Koo, H. -J.; Whangbo, M. -H.; Kennedy, B. J.
  • Journal of Solid State Chemistry, Vol. 136, Issue 2
  • DOI: 10.1006/jssc.1997.7705

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore Nd 2 Ir 2 O 7
journal, July 2015


Epitaxial crystals of Bi 2 Pt 2 O 7 pyrochlore through the transformation of δ –Bi 2 O 3 fluorite
journal, March 2015

  • Gutiérrez–Llorente, Araceli; Joress, Howie; Woll, Arthur
  • APL Materials, Vol. 3, Issue 3
  • DOI: 10.1063/1.4908103

Spin-orbit interaction and phase coherence in lithographically defined bismuth wires
journal, May 2011


Longer-range lattice anisotropy strongly competing with spin-orbit interactions in pyrochlore iridates
journal, March 2014


Metal–Insulator Transitions in Pyrochlore Oxides Ln 2 Ir 2 O 7
journal, September 2011

  • Matsuhira, Kazuyuki; Wakeshima, Makoto; Hinatsu, Yukio
  • Journal of the Physical Society of Japan, Vol. 80, Issue 9
  • DOI: 10.1143/JPSJ.80.094701

Disordered electronic systems
journal, April 1985


Optical evidence for a Weyl semimetal state in pyrochlore Eu 2 Ir 2 O 7
journal, December 2015


Cation antisite disorder in uranium-doped gadolinium zirconate pyrochlores
journal, September 2014


Oxygen content tailored magnetic and electronic properties in cobaltite double perovskite thin films
journal, February 2017

  • Harrell, Zach; Enriquez, Erik; Chen, Aiping
  • Applied Physics Letters, Vol. 110, Issue 9
  • DOI: 10.1063/1.4977026

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009


Topological insulators and metal-insulator transition in the pyrochlore iridates
journal, August 2010


Infrared study of the electronic structure of the metallic pyrochlore iridate Bi 2 Ir 2 O 7
journal, May 2013


Emergent Topological Phenomena in Thin Films of Pyrochlore Iridates
journal, June 2014


Spin and phase coherence measured by antilocalization in n -InSb thin films
journal, February 2009


Magnetic order, spin dynamics and transport properties of the pyrochlore iridate Y2Ir2O7
journal, February 2014


Epitaxial growth of iridate pyrochlore Nd2Ir2O7 films
journal, February 2016

  • Gallagher, J. C.; Esser, B. D.; Morrow, R.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep22282

Continuous transition between antiferromagnetic insulator and paramagnetic metal in the pyrochlore iridate Eu 2 Ir 2 O 7
journal, June 2012


Metal–Insulator Transition in Pyrochlore Iridates Ln 2 Ir 2 O 7 ( Ln = Nd, Sm, and Eu)
journal, April 2007

  • Matsuhira, Kazuyuki; Wakeshima, Makoto; Nakanishi, Ryo
  • Journal of the Physical Society of Japan, Vol. 76, Issue 4
  • DOI: 10.1143/JPSJ.76.043706

Comparative study of low-temperature x-ray diffraction experiments on R 2 Ir 2 O 7 ( R = Nd , Eu, and Pr)
journal, December 2014


Weyl Mott Insulator
journal, January 2016

  • Morimoto, Takahiro; Nagaosa, Naoto
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep19853

The electronic structure of iridium and its oxides: The electronic structure of iridium and its oxides
journal, December 2015

  • Pfeifer, Verena; Jones, Travis E.; Velasco Vélez, Juan J.
  • Surface and Interface Analysis, Vol. 48, Issue 5
  • DOI: 10.1002/sia.5895

First-principles calculations for defects and impurities: Applications to III-nitrides
journal, April 2004

  • Van de Walle, Chris G.; Neugebauer, Jörg
  • Journal of Applied Physics, Vol. 95, Issue 8
  • DOI: 10.1063/1.1682673

Oxygen vacancy-driven evolution of structural and electrical properties in SrFeO3−δ thin films and a method of stabilization
journal, October 2016

  • Enriquez, Erik; Chen, Aiping; Harrell, Zach
  • Applied Physics Letters, Vol. 109, Issue 14
  • DOI: 10.1063/1.4964384

Structure and magnetic properties of the pyrochlore iridate Y 2 Ir 2 O 7
journal, June 2012


Magnetic order in the pyrochlore iridates A 2 Ir 2 O 7 ( A = Y, Yb)
journal, July 2012


Tuning electronic structure via epitaxial strain in Sr 2 IrO 4 thin films
journal, April 2013

  • Nichols, J.; Terzic, J.; Bittle, E. G.
  • Applied Physics Letters, Vol. 102, Issue 14
  • DOI: 10.1063/1.4801877

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Variation of Charge Dynamics in the Course of Metal-Insulator Transition for Pyrochlore-Type Nd 2 Ir 2 O 7
journal, September 2012


Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4
journal, August 2008


All-in-all-out magnetic domain size in pyrochlore iridate thin films as probed by local magnetotransport
journal, January 2016

  • Fujita, T. C.; Uchida, M.; Kozuka, Y.
  • Applied Physics Letters, Vol. 108, Issue 2
  • DOI: 10.1063/1.4939742

Enhanced weak ferromagnetism and conductivity in hole-doped pyrochlore iridate Y 2 Ir 2 O 7
journal, August 2014


Strong oxygen pressure dependence of ferroelectricity in BaTiO 3 /SrRuO 3 /SrTiO 3 epitaxial heterostructures
journal, September 2013

  • Chen, A. P.; Khatkhatay, F.; Zhang, W.
  • Journal of Applied Physics, Vol. 114, Issue 12
  • DOI: 10.1063/1.4821643

Local Character of Many-Body Effects in X-Ray Photoemission from Transition-Metal Compounds: Na x W O 3
journal, March 1975


Why is lead dioxide metallic?
journal, August 2005


In Situ Observation of Surface Species on Iridium Oxide Nanoparticles during the Oxygen Evolution Reaction
journal, May 2014

  • Sanchez Casalongue, Hernan G.; Ng, May Ling; Kaya, Sarp
  • Angewandte Chemie International Edition, Vol. 53, Issue 28
  • DOI: 10.1002/anie.201402311

Crystal structure and disorder of the fast oxide-ion conductor cubic Bi2O3
journal, September 2003


Time-reversal symmetry breaking and spontaneous Hall effect without magnetic dipole order
journal, December 2009

  • Machida, Yo; Nakatsuji, Satoru; Onoda, Shigeki
  • Nature, Vol. 463, Issue 7278
  • DOI: 10.1038/nature08680

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Chemical potential dependence of defect formation energies in GaAs: Application to Ga self-diffusion
journal, October 1991


Spin-Orbit Interaction and Magnetoresistance in the Two Dimensional Random System
journal, February 1980

  • Hikami, S.; Larkin, A. I.; Nagaoka, Y.
  • Progress of Theoretical Physics, Vol. 63, Issue 2
  • DOI: 10.1143/PTP.63.707

Localization and electron-interaction effects in a two-dimensional metal with strong spin-orbit scattering: Pd films
journal, January 1984


Zero bias anomaly in tunnel resistance and electron-electron interaction
journal, April 1979


Magnetotransport and induced superconductivity in Bi based three-dimensional topological insulators
journal, December 2012

  • Veldhorst, M.; Snelder, M.; Hoek, M.
  • physica status solidi (RRL) - Rapid Research Letters, Vol. 7, Issue 1-2
  • DOI: 10.1002/pssr.201206408

Recent progress on correlated electron systems with strong spin–orbit coupling
journal, August 2016


Magnetic order in the pyrochlore iridate Nd 2 Ir 2 O 7 probed by muon spin relaxation
journal, August 2013


Magnetic transition, long-range order, and moment fluctuations in the pyrochlore iridate Eu 2 Ir 2 O 7
journal, May 2011


Magnetic order and the electronic ground state in the pyrochlore iridate Nd 2 Ir 2 O 7
journal, May 2012


Weak magnetic transitions in pyrochlore Bi 2 Ir 2 O 7
journal, May 2013


Strong magnetic instability in correlated metallic Bi 2 Ir 2 O 7
journal, July 2012


The influence of Sn doping on the growth of In2O3 on Y-stabilized ZrO2(100) by oxygen plasma assisted molecular beam epitaxy
journal, July 2009

  • Bourlange, A.; Payne, D. J.; Palgrave, R. G.
  • Journal of Applied Physics, Vol. 106, Issue 1
  • DOI: 10.1063/1.3153966

Field-induced quantum metal–insulator transition in the pyrochlore iridate Nd2Ir2O7
journal, November 2015

  • Tian, Zhaoming; Kohama, Yoshimitsu; Tomita, Takahiro
  • Nature Physics, Vol. 12, Issue 2
  • DOI: 10.1038/nphys3567

Pressure-tuned insulator to metal transition in Eu 2 Ir 2 O 7
journal, May 2012


Mobile metallic domain walls in an all-in-all-out magnetic insulator
journal, October 2015


Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates
journal, May 2011


All-in-all-out magnetic domain wall conduction in a pyrochlore iridate heterointerface
journal, February 2016


Works referencing / citing this record:

Spectroscopic Studies on the Metal-Insulator Transition Mechanism in Correlated Materials
journal, May 2018


Reduced Transition Temperature in Al:ZnO/VO2 Based Multi-Layered Device for low Powered Smart Window Application
journal, February 2020

  • Behera, Makhes K.; Williams, Leslie C.; Pradhan, Sangram K.
  • Scientific Reports, Vol. 10, Issue 1
  • DOI: 10.1038/s41598-020-58698-w

Strain-engineering of charge transport in the correlated Dirac semimetal of perovskite CaIrO 3 thin films
journal, August 2019

  • Masuko, M.; Fujioka, J.; Nakamura, M.
  • APL Materials, Vol. 7, Issue 8
  • DOI: 10.1063/1.5109582

Influence of electronic structure parameters on the electrical transport and magnetic properties of Y 2− x Bi x Ir 2 O 7 pyrochlore iridates
journal, October 2019

  • Dwivedi, Vinod Kumar; Mukhopadhyay, Soumik
  • Journal of Applied Physics, Vol. 126, Issue 16
  • DOI: 10.1063/1.5125254

Topological properties and functionalities in oxide thin films and interfaces
journal, March 2018

  • Uchida, Masaki; Kawasaki, Masashi
  • Journal of Physics D: Applied Physics, Vol. 51, Issue 14
  • DOI: 10.1088/1361-6463/aaaf00

Possible scale invariant linear magnetoresistance in pyrochlore iridates Bi 2 Ir 2 O 7
journal, November 2019


Unconventional anomalous Hall effect from antiferromagnetic domain walls of N d 2 I r 2 O 7 thin films
journal, September 2018


Robust pinning of magnetic moments in pyrochlore iridates
text, January 2017


Topological Properties and Functionalities in Oxide Thin Films and Interfaces
text, January 2018