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Title: Stabilization of Polar Nanoregions in Pb-free Ferroelectrics

Abstract

In this study, the formation of polar nanoregions through solid-solution additions is known to enhance significantly the functional properties of ferroelectric materials. Despite considerable progress in characterizing the microscopic behavior of polar nanoregions (PNR), understanding their real-space atomic structure and dynamics of their formation remains a considerable challenge. Here, using the method of dynamic pair distribution function, we provide direct insights into the role of solid-solution additions towards the stabilization of polar nanoregions in the Pb-free ferroelectric of Ba(Zr,Ti)O3. It is shown that for an optimum level of substitution of Ti by larger Zr ions, the dynamics of atomic displacements for ferroelectric polarization are slowed sufficiently below THz frequencies, which leads to increased local correlation among dipoles within PNRs. The dynamic pair distribution function technique demonstrates a unique capability to obtain insights into locally correlated atomic dynamics in disordered materials, including new Pb-free ferroelectrics, which is necessary to understand and control their functional properties.

Authors:
 [1];  [2];  [2];  [1];  [3];  [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4];  [5]
  1. City Univ. of Hong Kong, Kowloon Tong (Hong Kong SAR)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Oak Ridge, TN (United States)
  3. Technische Univ. Darmstadt, Darmstadt (Germany)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Aarhus Univ., Aarhus C (Denmark); Lund Univ., Lund (Sweden)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1440833
Alternate Identifier(s):
OSTI ID: 1437680
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 20; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., and Jorgensen, M. R. V. Stabilization of Polar Nanoregions in Pb-free Ferroelectrics. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.207603.
Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., & Jorgensen, M. R. V. Stabilization of Polar Nanoregions in Pb-free Ferroelectrics. United States. doi:10.1103/PhysRevLett.120.207603.
Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., and Jorgensen, M. R. V. Fri . "Stabilization of Polar Nanoregions in Pb-free Ferroelectrics". United States. doi:10.1103/PhysRevLett.120.207603. https://www.osti.gov/servlets/purl/1440833.
@article{osti_1440833,
title = {Stabilization of Polar Nanoregions in Pb-free Ferroelectrics},
author = {Pramanick, A. and Dmowski, Wojciech and Egami, Takeshi and Budisuharto, A. Setiadi and Weyland, F. and Novak, N. and Christianson, Andrew D. and Borreguero, J. M. and Abernathy, Douglas L. and Jorgensen, M. R. V.},
abstractNote = {In this study, the formation of polar nanoregions through solid-solution additions is known to enhance significantly the functional properties of ferroelectric materials. Despite considerable progress in characterizing the microscopic behavior of polar nanoregions (PNR), understanding their real-space atomic structure and dynamics of their formation remains a considerable challenge. Here, using the method of dynamic pair distribution function, we provide direct insights into the role of solid-solution additions towards the stabilization of polar nanoregions in the Pb-free ferroelectric of Ba(Zr,Ti)O3. It is shown that for an optimum level of substitution of Ti by larger Zr ions, the dynamics of atomic displacements for ferroelectric polarization are slowed sufficiently below THz frequencies, which leads to increased local correlation among dipoles within PNRs. The dynamic pair distribution function technique demonstrates a unique capability to obtain insights into locally correlated atomic dynamics in disordered materials, including new Pb-free ferroelectrics, which is necessary to understand and control their functional properties.},
doi = {10.1103/PhysRevLett.120.207603},
journal = {Physical Review Letters},
number = 20,
volume = 120,
place = {United States},
year = {2018},
month = {5}
}

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Figures / Tables:

Figure 1 Figure 1: (a) Phase diagram of Ba(ZrxTi1-x)O3. The compositions used for the current study are shown by dotted lines. (b) Dielectric permittivity $ε_{r}$ as a function of temperature for different x. (c) Comparison of P-E hysteresis loops for x = 0.10 and x = 0.15. The decrease in coercive 11more » fields at 30 °C is likely due to thermally facilitated initiation of domain-wall motion (d) 1/$ε_{r}$ for x = 0.15 and x = 0.10; the scales for the plots are normalized for comparison. The curves are compared to expected behavior for the two exponents. (e) Pr and Pmax for x = 0.15 display nonzero values above TC (f) Change in temperature $Δ$T due to electrocaloric effect for x = 0.15. The temperature of maximum $Δ$T as a function of the applied electric field is shown in the inset.« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.