skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Complex magnetic order in nickelate slabs

Abstract

Here, magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO 3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system—NdNiO 3 slabs embedded in a non-magnetic NdGaO 3 matrix—and use polarized resonant X-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighbouring NiO 6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [5];  [5];  [6];  [7];  [8]; ORCiD logo [9]; ORCiD logo [9];  [5];  [5]; ORCiD logo [5];  [5];  [10];  [11];  [7];  [12];  [5] more »; ORCiD logo [5] « less
  1. Max Planck Institute for Solid State Research, Stuttgart (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Menlo Park, CA (United States)
  2. Univ. of British Columbia, Vancouver, BC (Canada); Univ. of Saskatchewan, Saskatoon, SK (Canada)
  3. Max Planck Institute for Solid State Research, Stuttgart (Germany); Chinese Academy of Sciences, Ningbo (China)
  4. Max Planck Institute for Solid State Research, Stuttgart (Germany); Wilhelm-Conrad-Rontgen-Campus BESSY II, Berlin (Germany)
  5. Max Planck Institute for Solid State Research, Stuttgart (Germany)
  6. Univ. of California, Berkeley, CA (United States); Univ. of California San Diego, La Jolla, CA (United States)
  7. Univ. of Geneva, Geneva (Switzerland)
  8. Univ. of Geneva, Geneva (Switzerland); Univ. of Zurich, Zurich (Switzerland)
  9. Canadian Light Sources, Inc., Saskatoon, SK (Canada)
  10. Max Planck Institute for Solid State Research, Stuttgart (Germany); Eberhard Karls Univ. Tubingen, Tubingen (Germany)
  11. Max Planck Institute for Solid State Research, Stuttgart (Germany); Karlsruher Institut fur Technologie, Eggenstein-Leopoldshafen (Germany)
  12. Univ. of British Columbia, Vancouver, BC (Canada)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490656
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 14; Journal Issue: 11; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Hepting, M., Green, R. J., Zhong, Z., Bluschke, M., Suyolcu, Y. E., Macke, S., Frano, A., Catalano, S., Gibert, M., Sutarto, R., He, F., Cristiani, G., Logvenov, G., Wang, Y., van Aken, P. A., Hansmann, P., Le Tacon, M., Triscone, J. -M., Sawatzky, G. A., Keimer, B., and Benckiser, E. Complex magnetic order in nickelate slabs. United States: N. p., 2018. Web. doi:10.1038/s41567-018-0218-5.
Hepting, M., Green, R. J., Zhong, Z., Bluschke, M., Suyolcu, Y. E., Macke, S., Frano, A., Catalano, S., Gibert, M., Sutarto, R., He, F., Cristiani, G., Logvenov, G., Wang, Y., van Aken, P. A., Hansmann, P., Le Tacon, M., Triscone, J. -M., Sawatzky, G. A., Keimer, B., & Benckiser, E. Complex magnetic order in nickelate slabs. United States. doi:10.1038/s41567-018-0218-5.
Hepting, M., Green, R. J., Zhong, Z., Bluschke, M., Suyolcu, Y. E., Macke, S., Frano, A., Catalano, S., Gibert, M., Sutarto, R., He, F., Cristiani, G., Logvenov, G., Wang, Y., van Aken, P. A., Hansmann, P., Le Tacon, M., Triscone, J. -M., Sawatzky, G. A., Keimer, B., and Benckiser, E. Mon . "Complex magnetic order in nickelate slabs". United States. doi:10.1038/s41567-018-0218-5. https://www.osti.gov/servlets/purl/1490656.
@article{osti_1490656,
title = {Complex magnetic order in nickelate slabs},
author = {Hepting, M. and Green, R. J. and Zhong, Z. and Bluschke, M. and Suyolcu, Y. E. and Macke, S. and Frano, A. and Catalano, S. and Gibert, M. and Sutarto, R. and He, F. and Cristiani, G. and Logvenov, G. and Wang, Y. and van Aken, P. A. and Hansmann, P. and Le Tacon, M. and Triscone, J. -M. and Sawatzky, G. A. and Keimer, B. and Benckiser, E.},
abstractNote = {Here, magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system—NdNiO3 slabs embedded in a non-magnetic NdGaO3 matrix—and use polarized resonant X-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighbouring NiO6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.},
doi = {10.1038/s41567-018-0218-5},
journal = {Nature Physics},
number = 11,
volume = 14,
place = {United States},
year = {2018},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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

Charge Disproportionation without Charge Transfer in the Rare-Earth-Element Nickelates as a Possible Mechanism for the Metal-Insulator Transition
journal, March 2014


Landau Theory of Charge and Spin Ordering in the Nickelates
journal, January 2011


Dimensionality Control of Electronic Phase Transitions in Nickel-Oxide Superlattices
journal, May 2011


Orbital Control of Noncollinear Magnetic Order in Nickel Oxide Heterostructures
journal, September 2013


Multiferroicity in Rare-Earth Nickelates R NiO 3
journal, October 2009


Transfer of Magnetic Order and Anisotropy through Epitaxial Integration of 3 d and 4 f Spin Systems
journal, May 2017


Strain and composition dependence of orbital polarization in nickel oxide superlattices
journal, September 2013


Dynamical Effects in Resonant X-Ray Diffraction
journal, September 2016


Complete phase diagram of rare-earth nickelates from first-principles
journal, April 2017

  • Varignon, Julien; Grisolia, Mathieu N.; Íñiguez, Jorge
  • npj Quantum Materials, Vol. 2, Issue 1
  • DOI: 10.1038/s41535-017-0024-9

Role of magnetic and orbital ordering at the metal-insulator transition in NdNiO 3
journal, March 2006


Site-Selective Mott Transition in Rare-Earth-Element Nickelates
journal, October 2012


Spin and charge ordering in self-doped Mott insulators
journal, May 2000


On the magnetic structure of DyNiO3
journal, July 2009

  • Muñoz, A.; Alonso, J. A.; Martínez-Lope, M. J.
  • Journal of Solid State Chemistry, Vol. 182, Issue 7
  • DOI: 10.1016/j.jssc.2009.05.013

Theoretical Form Factor, Attenuation, and Scattering Tabulation for Z =1–92 from E =1–10 eV to E =0.4–1.0 MeV
journal, January 1995

  • Chantler, C. T.
  • Journal of Physical and Chemical Reference Data, Vol. 24, Issue 1
  • DOI: 10.1063/1.555974

Structure and charge order in the antiferromagnetic band-insulating phase of NdNiO 3
journal, April 2009


Sudden Appearance of an Unusual Spin Density Wave At the Metal-Insulator Transition in the Perovskites RNiO 3 (R = Pr, Nd)
journal, October 1992

  • García-Muñoz, J. L.; Rodríguez-Carvajal, J.; Lacorre, P.
  • Europhysics Letters (EPL), Vol. 20, Issue 3
  • DOI: 10.1209/0295-5075/20/3/009

Tailoring the electronic transitions of NdNiO 3 films through (111) pc oriented interfaces
journal, June 2015

  • Catalano, S.; Gibert, M.; Bisogni, V.
  • APL Materials, Vol. 3, Issue 6
  • DOI: 10.1063/1.4919803

Induced noncollinear magnetic order of Nd 3 + in Nd Ni O 3 observed by resonant soft x-ray diffraction
journal, March 2008


Progress in perovskite nickelate research
journal, July 2008


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling
journal, March 2016

  • Liao, Z.; Huijben, M.; Zhong, Z.
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4579

Renormalization of effective interactions in a negative charge transfer insulator
journal, November 2017


Interplay between breathing mode distortion and magnetic order in rare-earth nickelates R NiO 3 within DFT + U
journal, October 2017


Mapping chemical and bonding information using multivariate analysis of electron energy-loss spectrum images
journal, October 2006


Bond disproportionation and dynamical charge fluctuations in the perovskite rare-earth nickelates
journal, November 2016


Low-energy description of the metal-insulator transition in the rare-earth nickelates
journal, February 2015


Charge Disproportionation in R NiO 3 Perovskites: Simultaneous Metal-Insulator and Structural Transition in YNiO 3
journal, May 1999

  • Alonso, J. A.; García-Muñoz, J. L.; Fernández-Díaz, M. T.
  • Physical Review Letters, Vol. 82, Issue 19
  • DOI: 10.1103/PhysRevLett.82.3871

2D materials and van der Waals heterostructures
journal, July 2016


Exchange bias in LaNiO3–LaMnO3 superlattices
journal, January 2012

  • Gibert, Marta; Zubko, Pavlo; Scherwitzl, Raoul
  • Nature Materials, Vol. 11, Issue 3
  • DOI: 10.1038/nmat3224

Effects of Double Exchange in Magnetic Crystals
journal, April 1960


X-Ray Resonance Exchange Scattering
journal, September 1988


Oxygen octahedra picker: A software tool to extract quantitative information from STEM images
journal, September 2016


Orbital reflectometry of oxide heterostructures
journal, February 2011

  • Benckiser, Eva; Haverkort, Maurits W.; Brück, Sebastian
  • Nature Materials, Vol. 10, Issue 3
  • DOI: 10.1038/nmat2958

Hybridization-controlled charge transfer and induced magnetism at correlated oxide interfaces
journal, January 2016

  • Grisolia, M. N.; Varignon, J.; Sanchez-Santolino, G.
  • Nature Physics, Vol. 12, Issue 5
  • DOI: 10.1038/nphys3627

Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates
journal, October 2016

  • Bisogni, Valentina; Catalano, Sara; Green, Robert J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13017

Tunable Charge and Spin Order in PrNiO 3 Thin Films and Superlattices
journal, November 2014


Direct Observation of Charge Order in an Epitaxial NdNiO 3 Film
journal, March 2002


Symmetry analysis of magneto-optical effects: The case of x-ray diffraction and x-ray absorption at the transition metal L 2 , 3 edge
journal, September 2010


Antiferromagnetic correlations in the metallic strongly correlated transition metal oxide LaNiO3
journal, January 2018