Multiferroic behavior in EuTiO3 films constrained by symmetry

Ryan, P. J.; Sterbinsky, G. E.; Choi, Y.; Woicik, J. C.; Zhu, Leyi; Jiang, J. S.; Lee, J. -H.; Schlom, D. G.; Birol, T.; Brown, S. D.; Thompson, P. B. J.; Normile, P. S.; Lang, J.; Kim, J. -W.

doi:10.1103/physrevb.101.180409

Title: Multiferroic behavior in EuTiO₃ films constrained by symmetry

Abstract

We have elucidated the spin, lattice, charge, and orbital coupling mechanism underlying the multiferroic character in tensile-strained EuTiO₃ films. Symmetry determined by oxygen octahedral tilting shapes the hybridization between the Eu 4f and the Ti 3d orbitals, and this inhibits predicted Ti displacement proper ferroelectricity. Instead, phonon softening emerges at low temperatures within the pseudocube (110) plane, orthogonal to the anticipated ferroelectric polarization symmetry. Additionally, the magnetic anisotropy is determined by orbital distortion through hybridization between the Ti 3d and the typically isotropic Eu²⁺ 4f states. Here, this unique scenario demonstrates the critical role symmetry plays in the coupling of order parameters defining multiferroic behavior.

Authors:

Ryan, P. J. ^[1]; Sterbinsky, G. E. ^[2];

^[2]; Woicik, J. C. ^[3]; Zhu, Leyi ^[2]; Jiang, J. S. ^[2]; Lee, J. -H. ^[4]; Schlom, D. G. ^[5];

^[6]; Brown, S. D. ^[7]; Thompson, P. B. J. ^[7];

^[8]; Lang, J. ^[2];

^[2]

Argonne National Laboratory (ANL), Argonne, IL (United States); Dublin City University (Ireland)
Argonne National Laboratory (ANL), Argonne, IL (United States)
National Institute of Standards and Technology, Gaithersburg, MD (United States)
Cornell University, Ithaca, NY (United States)
Cornell University, Ithaca, NY (United States); Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY (United States)
University of Minnesota, Minneapolis, MN (United States). Department of Chemical Engineering and Materials Science
University of Liverpool (United Kingdom)
Universidad de Castilla-La Mancha, Ciudad Real (Spain)

Publication Date:: Fri May 29 00:00:00 EDT 2020

Research Org.:: Univ. of Minnesota, Minneapolis, MN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1657858

Alternate Identifier(s):: OSTI ID: 1756928

Grant/Contract Number:: SC0016371; AC02-98CH10886; NNCI-1542081; AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 101; Journal Issue: 18; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Magnetic order; Magneto-dielectric effect; Ferromagnets; Multiferroics; X-ray resonant magnetic scattering

Citation Formats


                    Ryan, P. J., Sterbinsky, G. E., Choi, Y., Woicik, J. C., Zhu, Leyi, Jiang, J. S., Lee, J. -H., Schlom, D. G., Birol, T., Brown, S. D., Thompson, P. B. J., Normile, P. S., Lang, J., and Kim, J. -W. Multiferroic behavior in EuTiO3 films constrained by symmetry.  United States: N. p., 2020. 
Web.  doi:10.1103/physrevb.101.180409.

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                    Ryan, P. J., Sterbinsky, G. E., Choi, Y., Woicik, J. C., Zhu, Leyi, Jiang, J. S., Lee, J. -H., Schlom, D. G., Birol, T., Brown, S. D., Thompson, P. B. J., Normile, P. S., Lang, J., & Kim, J. -W. Multiferroic behavior in EuTiO3 films constrained by symmetry.  United States.  https://doi.org/10.1103/physrevb.101.180409

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                    Ryan, P. J., Sterbinsky, G. E., Choi, Y., Woicik, J. C., Zhu, Leyi, Jiang, J. S., Lee, J. -H., Schlom, D. G., Birol, T., Brown, S. D., Thompson, P. B. J., Normile, P. S., Lang, J., and Kim, J. -W. Fri .  
"Multiferroic behavior in EuTiO3 films constrained by symmetry".  United States.  https://doi.org/10.1103/physrevb.101.180409.  https://www.osti.gov/servlets/purl/1657858.

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@article{osti_1657858,

  title        = {Multiferroic behavior in EuTiO3 films constrained by symmetry},

  author       = {Ryan, P. J. and Sterbinsky, G. E. and Choi, Y. and Woicik, J. C. and Zhu, Leyi and Jiang, J. S. and Lee, J. -H. and Schlom, D. G. and Birol, T. and Brown, S. D. and Thompson, P. B. J. and Normile, P. S. and Lang, J. and Kim, J. -W.},

  abstractNote = {We have elucidated the spin, lattice, charge, and orbital coupling mechanism underlying the multiferroic character in tensile-strained EuTiO3 films. Symmetry determined by oxygen octahedral tilting shapes the hybridization between the Eu 4f and the Ti 3d orbitals, and this inhibits predicted Ti displacement proper ferroelectricity. Instead, phonon softening emerges at low temperatures within the pseudocube (110) plane, orthogonal to the anticipated ferroelectric polarization symmetry. Additionally, the magnetic anisotropy is determined by orbital distortion through hybridization between the Ti 3d and the typically isotropic Eu2+ 4f states. Here, this unique scenario demonstrates the critical role symmetry plays in the coupling of order parameters defining multiferroic behavior.},

  doi          = {10.1103/physrevb.101.180409},

  journal      = {Physical Review B},

  number       = 18,

  volume       = 101,

  place        = {United States},

  year         = {Fri May 29 00:00:00 EDT 2020},

  month        = {Fri May 29 00:00:00 EDT 2020}

}

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Title: Multiferroic behavior in EuTiO3 films constrained by symmetry

Abstract

Citation Formats

Pre-edge fine structure of the 3d atom K x-ray absorption spectra and quantitative atomic structure determinations for ferroelectric perovskite structure crystals journal, October 1998

Quantum critical behavior of a magnetic quantum paraelectric journal, August 2012

Reversible control of magnetic interactions by electric field in a single-phase material journal, January 2013

Lattice instabilities in bulk EuTiO 3 journal, October 2013

Role of A -Site and B -Site Ions in Perovskite Ferroelectricity journal, August 2006

Why Are There so Few Magnetic Ferroelectrics? journal, July 2000

Strong Spin-Lattice Coupling Through Oxygen Octahedral Rotation in Divalent Europium Perovskites journal, November 2012

Polar metals by geometric design journal, April 2016

A strong ferroelectric ferromagnet created by means of spin–lattice coupling journal, August 2010

Coupling between magnetism and dielectric properties in quantum paraelectric EuTiO 3 journal, July 2001

Character of Order-Disorder and Displacive Components in Barium Titanate journal, July 2004

Structural control of magnetic anisotropy in a strain-driven multiferroic EuTiO 3 thin film journal, September 2013

Band Gap and Edge Engineering via Ferroic Distortion and Anisotropic Strain: The Case of SrTiO 3 journal, September 2011

Competing Structural Instabilities in Cubic Perovskites journal, March 1995

Group-Theoretical Analysis of Octahedral Tilting in Perovskites journal, December 1998

Origin of ferroelectricity in perovskite oxides journal, July 1992

X-ray resonance exchange scattering from ferromagnets: A new approach and its application to EuS journal, July 2002

Symmetric vs. asymmetric linear M-X-M linkages in molecules, polymers, and extended networks journal, April 1986

Emergent Superstructural Dynamic Order due to Competing Antiferroelectric and Antiferrodistortive Instabilities in Bulk EuTiO 3 journal, January 2013

Antiferromagnetic superexchange via 3 d states of titanium in EuTiO 3 as seen from hybrid Hartree-Fock density functional calculations journal, June 2011

Understanding and Revisiting Properties of EuTiO 3 Bulk Material and Films from First Principles journal, December 2012

Multiferroic quantum criticality journal, December 2018

Ferroelectric distortion in SrTiO 3 thin films on Si ( 001 ) by x-ray absorption fine structure spectroscopy: Experiment and first-principles calculations journal, April 2007

Magnetic scattering of x rays (invited) journal, April 1985

Electronic structure and magnetism of EuTiO 3 : a first-principles study journal, September 2007

Experimental evidence of thermal fluctuations on the x-ray absorption near-edge structure at the aluminum K edge journal, June 2012

Magnetic Structure of EuTiO 3 journal, March 1966

Revival of the magnetoelectric effect journal, April 2005

Origin of giant spin-lattice coupling and the suppression of ferroelectricity in EuTiO 3 from first principles journal, September 2013

Multiferroic and magnetoelectric materials journal, August 2006

Why Are There So Few Perovskite Ferroelectrics? journal, May 2013

Title: Multiferroic behavior in EuTiO₃ films constrained by symmetry

Pre-edge fine structure of the 3d atom K x-ray absorption spectra and quantitative atomic structure determinations for ferroelectric perovskite structure crystals
journal, October 1998

Quantum critical behavior of a magnetic quantum paraelectric
journal, August 2012

Reversible control of magnetic interactions by electric field in a single-phase material
journal, January 2013

Lattice instabilities in bulk EuTiO $_{3}$
journal, October 2013

Role of A -Site and B -Site Ions in Perovskite Ferroelectricity
journal, August 2006

Why Are There so Few Magnetic Ferroelectrics?
journal, July 2000

Strong Spin-Lattice Coupling Through Oxygen Octahedral Rotation in Divalent Europium Perovskites
journal, November 2012

Polar metals by geometric design
journal, April 2016

A strong ferroelectric ferromagnet created by means of spin–lattice coupling
journal, August 2010

Coupling between magnetism and dielectric properties in quantum paraelectric ${EuTiO}_{3}$
journal, July 2001

Character of Order-Disorder and Displacive Components in Barium Titanate
journal, July 2004

Structural control of magnetic anisotropy in a strain-driven multiferroic EuTiO $_{3}$ thin film
journal, September 2013

Band Gap and Edge Engineering via Ferroic Distortion and Anisotropic Strain: The Case of ${SrTiO}_{3}$
journal, September 2011

Competing Structural Instabilities in Cubic Perovskites
journal, March 1995

Group-Theoretical Analysis of Octahedral Tilting in Perovskites
journal, December 1998

Origin of ferroelectricity in perovskite oxides
journal, July 1992

X-ray resonance exchange scattering from ferromagnets: A new approach and its application to EuS
journal, July 2002

Symmetric vs. asymmetric linear M-X-M linkages in molecules, polymers, and extended networks
journal, April 1986

Emergent Superstructural Dynamic Order due to Competing Antiferroelectric and Antiferrodistortive Instabilities in Bulk ${EuTiO}_{3}$
journal, January 2013

Antiferromagnetic superexchange via $3 d$ states of titanium in EuTiO $_{3}$ as seen from hybrid Hartree-Fock density functional calculations
journal, June 2011

Understanding and Revisiting Properties of ${EuTiO}_{3}$ Bulk Material and Films from First Principles
journal, December 2012

Multiferroic quantum criticality
journal, December 2018

Ferroelectric distortion in ${SrTiO}_{3}$ thin films on $Si (001)$ by x-ray absorption fine structure spectroscopy: Experiment and first-principles calculations
journal, April 2007

Magnetic scattering of x rays (invited)
journal, April 1985

Electronic structure and magnetism of EuTiO ₃ : a first-principles study
journal, September 2007

Experimental evidence of thermal fluctuations on the x-ray absorption near-edge structure at the aluminum $K$ edge
journal, June 2012

Magnetic Structure of EuTiO ₃
journal, March 1966

Revival of the magnetoelectric effect
journal, April 2005

Origin of giant spin-lattice coupling and the suppression of ferroelectricity in EuTiO $_{3}$ from first principles
journal, September 2013

Multiferroic and magnetoelectric materials
journal, August 2006

Why Are There So Few Perovskite Ferroelectrics?
journal, May 2013