DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Observation of polar vortices in oxide superlattices

Abstract

The complex interplay of spin, charge, orbital and lattice degrees of freedom provides a plethora of exotic phases and physical phenomena. In recent years, complex spin topologies have emerged as a consequence of the electronic band structure and the interplay between spin and spin-orbit coupling in materials. Here we produce complex topologies of electrical polarization-namely, nanometre-scale vortex-antivortex (that is, clockwise-anticlockwise) arrays that are reminiscent of rotational spin topologies-by making use of the competition between charge, orbital and lattice degrees of freedom in superlattices of alternating lead titanate and strontium titanate layers. Atomic-scale mapping of the polar atomic displacements by scanning transmission electron microscopy reveals the presence of long-range ordered vortex-antivortex arrays that exhibit nearly continuous polarization rotation. Phase-field modelling confirms that the vortex array is the low-energy state for a range of superlattice periods. Within this range, the large gradient energy from the vortex structure is counterbalanced by the corresponding large reduction in overall electrostatic energy (which would otherwise arise from polar discontinuities at the lead titanate/strontium titanate interfaces) and the elastic energy associated with epitaxial constraints and domain formation. These observations have implications for the creation of new states of matter (such as dipolar skyrmions, hedgehog states) and associatedmore » phenomena in ferroic materials, such as electrically controllable chirality.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [3];  [5];  [5];  [3];  [3];  [6];  [1];  [2];  [7];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Univ. of California, Berkeley, CA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  7. Univ. of St. Andrews, Scotland (United Kingdom)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1530227
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 530; Journal Issue: 7589; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Yadav, A. K., Nelson, C. T., Hsu, S. L., Hong, Z., Clarkson, J. D., Schlepütz, C. M., Damodaran, A. R., Shafer, P., Arenholz, E., Dedon, L. R., Chen, D., Vishwanath, A., Minor, A. M., Chen, L. Q., Scott, J. F., Martin, L. W., and Ramesh, R. Observation of polar vortices in oxide superlattices. United States: N. p., 2016. Web. doi:10.1038/nature16463.
Yadav, A. K., Nelson, C. T., Hsu, S. L., Hong, Z., Clarkson, J. D., Schlepütz, C. M., Damodaran, A. R., Shafer, P., Arenholz, E., Dedon, L. R., Chen, D., Vishwanath, A., Minor, A. M., Chen, L. Q., Scott, J. F., Martin, L. W., & Ramesh, R. Observation of polar vortices in oxide superlattices. United States. https://doi.org/10.1038/nature16463
Yadav, A. K., Nelson, C. T., Hsu, S. L., Hong, Z., Clarkson, J. D., Schlepütz, C. M., Damodaran, A. R., Shafer, P., Arenholz, E., Dedon, L. R., Chen, D., Vishwanath, A., Minor, A. M., Chen, L. Q., Scott, J. F., Martin, L. W., and Ramesh, R. Wed . "Observation of polar vortices in oxide superlattices". United States. https://doi.org/10.1038/nature16463. https://www.osti.gov/servlets/purl/1530227.
@article{osti_1530227,
title = {Observation of polar vortices in oxide superlattices},
author = {Yadav, A. K. and Nelson, C. T. and Hsu, S. L. and Hong, Z. and Clarkson, J. D. and Schlepütz, C. M. and Damodaran, A. R. and Shafer, P. and Arenholz, E. and Dedon, L. R. and Chen, D. and Vishwanath, A. and Minor, A. M. and Chen, L. Q. and Scott, J. F. and Martin, L. W. and Ramesh, R.},
abstractNote = {The complex interplay of spin, charge, orbital and lattice degrees of freedom provides a plethora of exotic phases and physical phenomena. In recent years, complex spin topologies have emerged as a consequence of the electronic band structure and the interplay between spin and spin-orbit coupling in materials. Here we produce complex topologies of electrical polarization-namely, nanometre-scale vortex-antivortex (that is, clockwise-anticlockwise) arrays that are reminiscent of rotational spin topologies-by making use of the competition between charge, orbital and lattice degrees of freedom in superlattices of alternating lead titanate and strontium titanate layers. Atomic-scale mapping of the polar atomic displacements by scanning transmission electron microscopy reveals the presence of long-range ordered vortex-antivortex arrays that exhibit nearly continuous polarization rotation. Phase-field modelling confirms that the vortex array is the low-energy state for a range of superlattice periods. Within this range, the large gradient energy from the vortex structure is counterbalanced by the corresponding large reduction in overall electrostatic energy (which would otherwise arise from polar discontinuities at the lead titanate/strontium titanate interfaces) and the elastic energy associated with epitaxial constraints and domain formation. These observations have implications for the creation of new states of matter (such as dipolar skyrmions, hedgehog states) and associated phenomena in ferroic materials, such as electrically controllable chirality.},
doi = {10.1038/nature16463},
journal = {Nature (London)},
number = 7589,
volume = 530,
place = {United States},
year = {Wed Jan 27 00:00:00 EST 2016},
month = {Wed Jan 27 00:00:00 EST 2016}
}

Works referenced in this record:

The structure of SrRuO3 by time-of-flight neutron powder diffraction
journal, March 1989

  • Jones, C. W.; Battle, P. D.; Lightfoot, P.
  • Acta Crystallographica Section C Crystal Structure Communications, Vol. 45, Issue 3
  • DOI: 10.1107/S0108270188012077

Ferroelectricity in Ultrathin Perovskite Films
journal, June 2004

  • Fong, Dillon D.; Stephenson, G. Brian; Streiffer, Stephen K.
  • Science, Vol. 304, Issue 5677, p. 1650-1653
  • DOI: 10.1126/science.1098252

Direct Observation of Continuous Electric Dipole Rotation in Flux-Closure Domains in Ferroelectric Pb(Zr,Ti)O3
journal, March 2011


Effect of electrical boundary conditions on ferroelectric domain structures in thin films
journal, July 2002

  • Li, Y. L.; Hu, S. Y.; Liu, Z. K.
  • Applied Physics Letters, Vol. 81, Issue 3
  • DOI: 10.1063/1.1492025

Spontaneous Vortex Nanodomain Arrays at Ferroelectric Heterointerfaces
journal, February 2011

  • Nelson, Christopher T.; Winchester, Benjamin; Zhang, Yi
  • Nano Letters, Vol. 11, Issue 2
  • DOI: 10.1021/nl1041808

Epitaxial Pb ( Zr , Ti ) O 3 Ultrathin Films under Open-Circuit Electrical Boundary Conditions
journal, May 2011


Unusual phase transitions in ferroelectric nanodisks and nanorods
journal, December 2004

  • Naumov, Ivan I.; Bellaiche, L.; Fu, Huaxiang
  • Nature, Vol. 432, Issue 7018
  • DOI: 10.1038/nature03107

Original properties of dipole vortices in zero-dimensional ferroelectrics
journal, April 2008


Thermodynamic theory of PbTiO 3
journal, October 1987

  • Haun, M. J.; Furman, E.; Jang, S. J.
  • Journal of Applied Physics, Vol. 62, Issue 8
  • DOI: 10.1063/1.339293

Interface control of bulk ferroelectric polarization
journal, May 2012

  • Yu, P.; Luo, W.; Yi, D.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 25
  • DOI: 10.1073/pnas.1117990109

Ferroelectric Phase Transitions in Small Particles and Local Regions
journal, August 2013


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


Improper ferroelectricity in perovskite oxide artificial superlattices
journal, April 2008

  • Bousquet, Eric; Dawber, Matthew; Stucki, Nicolas
  • Nature, Vol. 452, Issue 7188
  • DOI: 10.1038/nature06817

Elastic energy release due to domain formation in the strained epitaxy of ferroelectric and ferroelastic films
journal, November 1993

  • Pompe, W.; Gong, X.; Suo, Z.
  • Journal of Applied Physics, Vol. 74, Issue 10
  • DOI: 10.1063/1.355215

Chiral Patterns of Tilting of Oxygen Octahedra in Zero-Dimensional Ferroelectrics and Multiferroics: A First Principle-Based Study
journal, May 2010


Low-dimensional ferroelectrics under different electrical and mechanical boundary conditions: Atomistic simulations
journal, December 2005


Landau Expansion for Ferroelectrics: Which Variable to Use?
journal, December 2008


Mesoscale flux-closure domain formation in single-crystal BaTiO3
journal, July 2011

  • McQuaid, R. G. P.; McGilly, L. J.; Sharma, P.
  • Nature Communications, Vol. 2, Article No. 404
  • DOI: 10.1038/ncomms1413

Metal-insulator transitions
journal, October 1998

  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039

The role of the background dielectric susceptibility in uniaxial ferroelectrics
journal, July 1986


Powder profile refinement of lead zirconate titanate at several temperatures. II. Pure PbTiO 3
journal, April 1978

  • Glazer, A. M.; Mabud, S. A.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 34, Issue 4
  • DOI: 10.1107/S0567740878004938

Interface Physics in Complex Oxide Heterostructures
journal, March 2011


Geometric frustration in compositionally modulated ferroelectrics
journal, February 2011

  • Choudhury, Narayani; Walizer, Laura; Lisenkov, Sergey
  • Nature, Vol. 470, Issue 7335
  • DOI: 10.1038/nature09752

Effect of “symmetry mismatch” on the domain structure of rhombohedral BiFeO 3 thin films
journal, May 2014

  • Chen, Z. H.; Damodaran, A. R.; Xu, R.
  • Applied Physics Letters, Vol. 104, Issue 18
  • DOI: 10.1063/1.4875801

Lattice effects in magnetoresistive manganese perovskites
journal, March 1998


Evidence for Pb-O Covalency in Tetragonal PbTiO 3
journal, November 2001


Electronic liquid-crystal phases of a doped Mott insulator
journal, June 1998

  • Kivelson, S. A.; Fradkin, E.; Emery, V. J.
  • Nature, Vol. 393, Issue 6685
  • DOI: 10.1038/31177

Whither the oxide interface
journal, January 2012

  • Chakhalian, J.; Millis, A. J.; Rondinelli, J.
  • Nature Materials, Vol. 11, Issue 2
  • DOI: 10.1038/nmat3225

Physics of thin-film ferroelectric oxides
journal, October 2005


Topological properties and dynamics of magnetic skyrmions
journal, December 2013


Giant piezoelectric resistance in ferroelectric tunnel junctions
journal, January 2009


Tilt engineering of spontaneous polarization and magnetization above 300 K in a bulk layered perovskite
journal, January 2015


Observation of a periodic array of flux-closure quadrants in strained ferroelectric PbTiO3 films
journal, April 2015


Atomistic theory of hybrid improper ferroelectricity in perovskites
journal, May 2014


Phase-Field Method of Phase Transitions/Domain Structures in Ferroelectric Thin Films: A Review
journal, June 2008


Emergent electrodynamics of skyrmions in a chiral magnet
journal, February 2012

  • Schulz, T.; Ritz, R.; Bauer, A.
  • Nature Physics, Vol. 8, Issue 4
  • DOI: 10.1038/nphys2231

Enhanced electric conductivity at ferroelectric vortex cores in BiFeO3
journal, November 2011

  • Balke, Nina; Winchester, Benjamin; Ren, Wei
  • Nature Physics, Vol. 8, Issue 1
  • DOI: 10.1038/nphys2132

Effect of substrate constraint on the stability and evolution of ferroelectric domain structures in thin films
journal, January 2002


Orbital Physics in Transition-Metal Oxides
journal, April 2000


Vortex ferroelectric domains
journal, August 2008


A modified Landau–Devonshire thermodynamic potential for strontium titanate
journal, June 2010

  • Sheng, G.; Li, Y. L.; Zhang, J. X.
  • Applied Physics Letters, Vol. 96, Issue 23
  • DOI: 10.1063/1.3442915

Strain Tuning of Ferroelectric Thin Films
journal, August 2007


Works referencing / citing this record:

Quantification of flexoelectricity in PbTiO3/SrTiO3 superlattice polar vortices using machine learning and phase-field modeling
journal, November 2017


Configurable topological textures in strain graded ferroelectric nanoplates
journal, January 2018


Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites
journal, December 2018


Scaling of domain cascades in stripe and skyrmion phases
journal, April 2019


Polar coupling enabled nonlinear optical filtering at MoS2/ferroelectric heterointerfaces
journal, March 2020


Thermooptical evidence of carrier-stabilized ferroelectricity in ultrathin electrodeless films
journal, May 2018


Studies of Multiferroic Palladium Perovskites
journal, February 2019


Electrospun CuO-Nanoparticles-Modified Polycaprolactone @Polypyrrole Fibers: An Application to Sensing Glucose in Saliva
journal, February 2018


Nanoscale design of polarization in ultrathin ferroelectric heterostructures
text, January 2017


Design and Manipulation of Ferroic Domains in Complex Oxide Heterostructures
text, January 2019