skip to main content

DOE PAGESDOE PAGES

Title: Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite

Magnetoelectrics offer tantalizing opportunities for devices coupling ferroelectricity and magnetism but remain difficult to realize. Breakthrough strategies could circumvent the mutually exclusive origins of magnetism and ferroelectricity by exploiting the interaction of multiple phonon modes in geometric improper and hybrid improper ferroelectrics. Yet, the proposed instability of a zone-boundary phonon mode, driving the emergence of ferroelectricity via coupling to a polar mode, remains to be directly observed. Here, we provide previously missing evidence for this scenario in the archetypal improper ferroelectric, yttrium manganite, through comprehensive scattering measurements of the atomic structure and phonons, supported with first-principles simulations. Our experiments and theoretical modeling resolve the origin of the unusual temperature dependence of the polarization and rule out a reported double-step ferroelectric transition. These results emphasize the critical role of phonon anharmonicity in rationalizing lattice instabilities in improper ferroelectrics and show that including these effects in simulations could facilitate the design of magnetoelectrics.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [4] ;  [4] ;  [5] ;  [3] ;  [1]
  1. Duke Univ., Durham, NC (United States). Dept. of Mechanical Engineering and Materials Science. Dept. of Physics; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  2. Duke Univ., Durham, NC (United States). Dept. of Mechanical Engineering and Materials Science. Dept. of Physics
  3. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357; AC02-05CH11231; SC0016166; DMR-1350002
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Duke Univ., Durham, NC (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ferroelectrics and multiferroics; phase transitions and critical phenomena
OSTI Identifier:
1427596
Alternate Identifier(s):
OSTI ID: 1461324

Bansal, Dipanshu, Niedziela, Jennifer L., Sinclair, Ryan, Garlea, V. Ovidiu, Abernathy, Douglas L., Chi, Songxue, Ren, Yang, Zhou, Haidong, and Delaire, Olivier. Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite. United States: N. p., Web. doi:10.1038/s41467-017-02309-2.
Bansal, Dipanshu, Niedziela, Jennifer L., Sinclair, Ryan, Garlea, V. Ovidiu, Abernathy, Douglas L., Chi, Songxue, Ren, Yang, Zhou, Haidong, & Delaire, Olivier. Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite. United States. doi:10.1038/s41467-017-02309-2.
Bansal, Dipanshu, Niedziela, Jennifer L., Sinclair, Ryan, Garlea, V. Ovidiu, Abernathy, Douglas L., Chi, Songxue, Ren, Yang, Zhou, Haidong, and Delaire, Olivier. 2018. "Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite". United States. doi:10.1038/s41467-017-02309-2. https://www.osti.gov/servlets/purl/1427596.
@article{osti_1427596,
title = {Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite},
author = {Bansal, Dipanshu and Niedziela, Jennifer L. and Sinclair, Ryan and Garlea, V. Ovidiu and Abernathy, Douglas L. and Chi, Songxue and Ren, Yang and Zhou, Haidong and Delaire, Olivier},
abstractNote = {Magnetoelectrics offer tantalizing opportunities for devices coupling ferroelectricity and magnetism but remain difficult to realize. Breakthrough strategies could circumvent the mutually exclusive origins of magnetism and ferroelectricity by exploiting the interaction of multiple phonon modes in geometric improper and hybrid improper ferroelectrics. Yet, the proposed instability of a zone-boundary phonon mode, driving the emergence of ferroelectricity via coupling to a polar mode, remains to be directly observed. Here, we provide previously missing evidence for this scenario in the archetypal improper ferroelectric, yttrium manganite, through comprehensive scattering measurements of the atomic structure and phonons, supported with first-principles simulations. Our experiments and theoretical modeling resolve the origin of the unusual temperature dependence of the polarization and rule out a reported double-step ferroelectric transition. These results emphasize the critical role of phonon anharmonicity in rationalizing lattice instabilities in improper ferroelectrics and show that including these effects in simulations could facilitate the design of magnetoelectrics.},
doi = {10.1038/s41467-017-02309-2},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

Works referenced in this record:

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

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

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998
  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Multiferroics progress and prospects in thin films
journal, January 2007
  • Ramesh, R.; Spaldin, Nicola A.
  • Nature Materials, Vol. 6, Issue 1, p. 21-29
  • DOI: 10.1038/nmat1805