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Title: Magnetism in iridate heterostructures leveraged by structural distortions

Abstract

Fundamental control of magnetic coupling through heterostructure morphology is a prerequisite for rational engineering of magnetic ground states. We report the tuning of magnetic interactions in superlattices composed of single and bilayers of SrIrO3 inter-spaced with SrTiO3 in analogy to the Ruddlesden-Popper series iridates. Magnetic scattering shows predominately c-axis antiferromagnetic orientation of the magnetic moments for the bilayer, as in Sr3Ir2O7. However, the magnetic excitation gap, measured by resonant inelastic x-ray scattering, is quite different between the two structures, evidencing a significant change in the stability of the competing magnetic phases. In contrast, the single layer iridate hosts a more bulk-like gap. We find these changes are driven by bending of the c-axis Ir-O-Ir bond, which is much weaker in the single layer, and subsequent local environment changes, evidenced through x-ray diffraction and magnetic excitation modeling. Our findings demonstrate how large changes in the magnetic interactions can be tailored and probed in spin-orbit coupled heterostructures by engineering subtle structural modulations.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [2];  [2];  [2];  [2];  [3]; ORCiD logo [4];  [4];  [4];  [4];  [4];  [4];  [4];  [5];  [6];  [7]; ORCiD logo [2] more »; ORCiD logo [1] « less
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
  3. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics; Univ. of Chinese Academy of Sciences, Beijing (China). School of Physical Sciences
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source; Dublin City Univ. (Ireland). School of Physical Sciences
  6. Charles Univ., Prague (Czech Republic). Dept. of Condensed Matter Physics
  7. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Tennessee, Knoxville, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Defense Advanced Research Projects Agency (DARPA) (United States); Ministry of Science and Technology (MOST) (China); Chinese Academy of Sciences (CAS) (China)
OSTI Identifier:
1501560
Alternate Identifier(s):
OSTI ID: 1515548
Report Number(s):
BNL-211401-2019-JAAM
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
SC0012704; AC02-06CH11357; HR0011-16-1-0005; 2015CB921302; XDB07020200
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; magnetic properties and materials; phase transitions and critical phenomena

Citation Formats

Meyers, D., Cao, Yue, Fabbris, G., Robinson, Neil J., Hao, Lin, Frederick, C., Traynor, N., Yang, J., Lin, Jiaqi, Upton, M. H., Casa, D., Kim, Jong-Woo, Gog, T., Karapetrova, E., Choi, Yongseong, Haskel, D., Ryan, P. J., Horak, Lukas, Liu, X., Liu, Jian, and Dean, M. P. M. Magnetism in iridate heterostructures leveraged by structural distortions. United States: N. p., 2019. Web. doi:10.1038/s41598-019-39422-9.
Meyers, D., Cao, Yue, Fabbris, G., Robinson, Neil J., Hao, Lin, Frederick, C., Traynor, N., Yang, J., Lin, Jiaqi, Upton, M. H., Casa, D., Kim, Jong-Woo, Gog, T., Karapetrova, E., Choi, Yongseong, Haskel, D., Ryan, P. J., Horak, Lukas, Liu, X., Liu, Jian, & Dean, M. P. M. Magnetism in iridate heterostructures leveraged by structural distortions. United States. doi:10.1038/s41598-019-39422-9.
Meyers, D., Cao, Yue, Fabbris, G., Robinson, Neil J., Hao, Lin, Frederick, C., Traynor, N., Yang, J., Lin, Jiaqi, Upton, M. H., Casa, D., Kim, Jong-Woo, Gog, T., Karapetrova, E., Choi, Yongseong, Haskel, D., Ryan, P. J., Horak, Lukas, Liu, X., Liu, Jian, and Dean, M. P. M. Tue . "Magnetism in iridate heterostructures leveraged by structural distortions". United States. doi:10.1038/s41598-019-39422-9. https://www.osti.gov/servlets/purl/1501560.
@article{osti_1501560,
title = {Magnetism in iridate heterostructures leveraged by structural distortions},
author = {Meyers, D. and Cao, Yue and Fabbris, G. and Robinson, Neil J. and Hao, Lin and Frederick, C. and Traynor, N. and Yang, J. and Lin, Jiaqi and Upton, M. H. and Casa, D. and Kim, Jong-Woo and Gog, T. and Karapetrova, E. and Choi, Yongseong and Haskel, D. and Ryan, P. J. and Horak, Lukas and Liu, X. and Liu, Jian and Dean, M. P. M.},
abstractNote = {Fundamental control of magnetic coupling through heterostructure morphology is a prerequisite for rational engineering of magnetic ground states. We report the tuning of magnetic interactions in superlattices composed of single and bilayers of SrIrO3 inter-spaced with SrTiO3 in analogy to the Ruddlesden-Popper series iridates. Magnetic scattering shows predominately c-axis antiferromagnetic orientation of the magnetic moments for the bilayer, as in Sr3Ir2O7. However, the magnetic excitation gap, measured by resonant inelastic x-ray scattering, is quite different between the two structures, evidencing a significant change in the stability of the competing magnetic phases. In contrast, the single layer iridate hosts a more bulk-like gap. We find these changes are driven by bending of the c-axis Ir-O-Ir bond, which is much weaker in the single layer, and subsequent local environment changes, evidenced through x-ray diffraction and magnetic excitation modeling. Our findings demonstrate how large changes in the magnetic interactions can be tailored and probed in spin-orbit coupled heterostructures by engineering subtle structural modulations.},
doi = {10.1038/s41598-019-39422-9},
journal = {Scientific Reports},
number = ,
volume = 9,
place = {United States},
year = {2019},
month = {3}
}

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Figures / Tables:

FIG. 1. FIG. 1.: a) Structure of the two SLs. White arrows show in- plane magnetic exchange pathways and the pink arrow shows the out-of-plane exchange in the bilayer. b) Left panel: Inte- grated intensity as a function of the azimuthal angle for the (0.5, 0.5, 9.5) magnetic re ection of themore » 2SIO/1STO sample are shown as red circles, along with the expected response for c-axis (solid grey line) and in-plane moment orientations (blue dashed lines). Right panel: Normalized magnetic Bragg peaks at maximum azimuth (90°) and where no intensity is expected for in-plane moments (7°).« less

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Works referenced in this record:

Giant spin gap and magnon localization in the disordered Heisenberg antiferromagnet Sr 2 Ir 1 x Ru x O 4
journal, March 2017


Decoupling Carrier Concentration and Electron-Phonon Coupling in Oxide Heterostructures Observed with Resonant Inelastic X-Ray Scattering
journal, December 2018


Correlation between metal-insulator transitions and structural distortions in high-electron-density SrTiO 3 quantum wells
journal, February 2014


Sr 2 IrO 4 : Gateway to cuprate superconductivity?
journal, June 2015


Anomalous magnetic and transport behavior in the magnetic insulator Sr 3 Ir 2 O 7
journal, December 2002


Dimensionality Driven Spin-Flop Transition in Layered Iridates
journal, July 2012


Structural and magnetic studies of Sr 2 IrO 4
journal, April 1994


Doping Evolution of Magnetic Order and Magnetic Excitations in ( Sr 1 x La x ) 3 Ir 2 O 7
journal, January 2017


Oxide Interfaces--An Opportunity for Electronics
journal, March 2010


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


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


Spin ordering and electronic texture in the bilayer iridate Sr 3 Ir 2 O 7
journal, September 2012


Structural investigation of the bilayer iridate Sr 3 Ir 2 O 7
journal, April 2016


Simple ways of determining perovskite structures
journal, November 1975


Engineering a Spin-Orbital Magnetic Insulator by Tailoring Superlattices
journal, June 2015


Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal Sr 2 IrO 4
journal, May 1998


Magnetic properties of bilayer Sr 3 Ir 2 O 7 : Role of epitaxial strain and oxygen vacancies
journal, January 2017


Quantifying octahedral rotations in strained perovskite oxide films
journal, July 2010


Dimensionality-strain phase diagram of strontium iridates
journal, March 2017


Canted antiferromagnetic ground state in Sr 3 Ir 2 O 7
journal, March 2007


Evidence of quantum dimer excitations in Sr 3 Ir 2 O 7
journal, July 2015


On the magnetic structure of Sr 3 Ir 2 O 7 : an x-ray resonant scattering study
journal, July 2012


Tuning Magnetic Coupling in Sr 2 IrO 4 Thin Films with Epitaxial Strain
journal, April 2014


Emergent phenomena at oxide interfaces
journal, January 2012

  • Hwang, H. Y.; Iwasa, Y.; Kawasaki, M.
  • Nature Materials, Vol. 11, Issue 2
  • DOI: 10.1038/nmat3223

Engineering 1D Quantum Stripes from Superlattices of 2D Layered Materials
journal, October 2016

  • Gruenewald, John H.; Kim, Jungho; Kim, Heung Sik
  • Advanced Materials, Vol. 29, Issue 1, Article No. 1603798
  • DOI: 10.1002/adma.201603798

Colloquium : Emergent properties in plane view: Strong correlations at oxide interfaces
journal, October 2014

  • Chakhalian, Jak; Freeland, John W.; Millis, Andrew J.
  • Reviews of Modern Physics, Vol. 86, Issue 4
  • DOI: 10.1103/RevModPhys.86.1189

Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers
journal, June 2015

  • Bogdanov, Nikolay A.; Katukuri, Vamshi M.; Romhányi, Judit
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8306

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


Metal versus insulator behavior in ultrathin SrTiO 3 -based heterostructures
journal, July 2016


Twisted Hubbard Model for Sr 2 IrO 4 : Magnetism and Possible High Temperature Superconductivity
journal, March 2011


Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet
journal, June 2014


Observation of a d-wave gap in electron-doped Sr2IrO4
journal, October 2015

  • Kim, Y. K.; Sung, N. H.; Denlinger, J. D.
  • Nature Physics, Vol. 12, Issue 1
  • DOI: 10.1038/nphys3503

Strain-induced nonsymmorphic symmetry breaking and removal of Dirac semimetallic nodal line in an orthoperovskite iridate
journal, February 2016


Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009


Structural refinement of Pbnm -type perovskite films from analysis of half-order diffraction peaks
journal, January 2017

  • Brahlek, M.; Choquette, A. K.; Smith, C. R.
  • Journal of Applied Physics, Vol. 121, Issue 4
  • DOI: 10.1063/1.4974362

Anisotropic softening of magnetic excitations in lightly electron-doped Sr 2 IrO 4
journal, June 2016


Persistent Paramagnons Deep in the Metallic Phase of Sr 2 x La x IrO 4
journal, September 2016


Anisotropic exchange and spin-wave damping in pure and electron-doped Sr 2 IrO 4
journal, August 2017


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.