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Collective nonlinear electric polarization via defect-driven local symmetry breaking

Journal Article · · Materials Horizons
DOI:https://doi.org/10.1039/c9mh00516a· OSTI ID:1840883
 [1];  [2];  [3];  [3];  [4];  [3];  [5];  [6];  [7];  [8];  [9];  [10];  [3];  [3];  [11];  [3]
  1. Australian National Univ., Canberra, ACT (Australia); Univ. of Warwick, Coventry (United States)
  2. Australian National Univ., Canberra, ACT (Australia); Australia Nuclear Science and Technology Organisation, Lucas Height, NSW (Australia); Univ. of Wollongong, North Wollongong, NSW (Australia)
  3. Australian National Univ., Canberra, ACT (Australia)
  4. Australian National Univ., Canberra, ACT (Australia); Australia Nuclear Science and Technology Organisation, Lucas Height, NSW (Australia)
  5. Univ. of New South Wales, Canberra, ACT (Australia)
  6. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
  7. Australia Nuclear Science and Technology Organisation, Lucas Height, NSW (Australia)
  8. Australian National Univ., Canberra, ACT (Australia). Centre for Advanced Microscopy
  9. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
  10. Xi'an Jiaotong Univ. (China). International Center for Dielectric Research, Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education
  11. The Univ. of New South Wales, Canberra, ACT (Australia)
+ Show Author Affiliations

In this work, we report the defect-mediated, abnormal non-linear polarization behavior observed in centrosymmetric rutile TiO2 where less than 1 at% of sterically mismatched Mg2+ ions are introduced to create ferroelectric-like polarization hysteresis loops. It is found that the defect cluster produces a dipole moment exceeding 6 Debye, with a rotatable component. Such a polarization is further enhanced by the displacement of neighboring Ti4+ ions. The coupling between such defect-driven symmetry-breaking regions generates a collective nonlinear electrical polarization state that persists to high temperatures. More importantly, an observation of abnormal bias shift of polarization hysteresis suggests an antiparallel alignment of certain dipoles frozen relative to the external poling electric field, which is associated with oxygen vacancy hopping. This result challenges the long-standing notion of parallel alignment of dipoles with the external electric field in ferroelectrics. Finally, this work also reveals an unexpected new form of non-linear dielectric polarization (non-ferroelectricity) in solid-state materials.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Laboratory Directed Research and Development (LDRD) Program; Australian Research Council (ARC); International Science and Technology Cooperation Program of China
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1840883
Report Number(s):
LA-UR--21-22624
Journal Information:
Materials Horizons, Journal Name: Materials Horizons Journal Issue: 8 Vol. 6; ISSN 2051-6347
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Progress, Outlook, and Challenges in Lead‐Free Energy‐Storage Ferroelectrics journal December 2019
High performance bulk photovoltaics in narrow-bandgap centrosymmetric ultrathin films journal January 2020

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