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Title: Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films

Abstract

It is well known that temperature- and electric-field-induced structural transitions in a polydomain ferroelectric can have profound effects on its electrothermal susceptibilities. Here, the role of such ferroelastic domains on the pyroelectric and electrocaloric response is experimentally investigated in thin films of the tetragonal ferroelectric PbZr0.2Ti0.8O3. By utilizing epitaxial strain, a rich set of ferroelastic polydomain states spanning a broad thermodynamic phase space are stabilized. Using temperature-dependent scanning-probe microscopy, X-ray diffraction, and high-frequency phase-sensitive pyroelectric measurements, the propensity of domains to reconfigure under a temperature perturbation is quantitatively studied. In turn, the “extrinsic” contributions to pyroelectricity exclusively due to changes between the ferroelastic domain population is elucidated as a function of epitaxial strain. Further, using highly sensitive thin-film resistive thermometry, direct electrocaloric temperature changes are measured on these polydomain thin films for the first time. The results demonstrate that temperature- and electric-field-driven domain interconversion under compressive strain diminish both the pyroelectric and the electrocaloric effects, while both these susceptibilities are enhanced due to the exact-opposite effect from the extrinsic contributions under tensile strain.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3];  [1];  [1];  [4];  [3]; ORCiD logo [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Div.
  3. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering
  4. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Div.
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences & Engineering Division (SC-22.2); US Army Research Office (ARO); National Science Foundation (NSF); USDOE
OSTI Identifier:
1526497
Alternate Identifier(s):
OSTI ID: 1493098
Grant/Contract Number:  
SC0012375; AC02-05CH11231; W911NF‐14‐1‐0104; OISE‐1545907; DGE 1752814; DMR‐1708615; DMR‐1608938; KC2202
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 5; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Pandya, Shishir, Velarde, Gabriel A., Gao, Ran, Everhardt, Arnoud S., Wilbur, Joshua D., Xu, Ruijuan, Maher, Josh T., Agar, Joshua C., Dames, Chris, and Martin, Lane W. Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films. United States: N. p., 2018. Web. doi:10.1002/adma.201803312.
Pandya, Shishir, Velarde, Gabriel A., Gao, Ran, Everhardt, Arnoud S., Wilbur, Joshua D., Xu, Ruijuan, Maher, Josh T., Agar, Joshua C., Dames, Chris, & Martin, Lane W. Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films. United States. doi:10.1002/adma.201803312.
Pandya, Shishir, Velarde, Gabriel A., Gao, Ran, Everhardt, Arnoud S., Wilbur, Joshua D., Xu, Ruijuan, Maher, Josh T., Agar, Joshua C., Dames, Chris, and Martin, Lane W. Wed . "Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films". United States. doi:10.1002/adma.201803312. https://www.osti.gov/servlets/purl/1526497.
@article{osti_1526497,
title = {Understanding the Role of Ferroelastic Domains on the Pyroelectric and Electrocaloric Effects in Ferroelectric Thin Films},
author = {Pandya, Shishir and Velarde, Gabriel A. and Gao, Ran and Everhardt, Arnoud S. and Wilbur, Joshua D. and Xu, Ruijuan and Maher, Josh T. and Agar, Joshua C. and Dames, Chris and Martin, Lane W.},
abstractNote = {It is well known that temperature- and electric-field-induced structural transitions in a polydomain ferroelectric can have profound effects on its electrothermal susceptibilities. Here, the role of such ferroelastic domains on the pyroelectric and electrocaloric response is experimentally investigated in thin films of the tetragonal ferroelectric PbZr0.2Ti0.8O3. By utilizing epitaxial strain, a rich set of ferroelastic polydomain states spanning a broad thermodynamic phase space are stabilized. Using temperature-dependent scanning-probe microscopy, X-ray diffraction, and high-frequency phase-sensitive pyroelectric measurements, the propensity of domains to reconfigure under a temperature perturbation is quantitatively studied. In turn, the “extrinsic” contributions to pyroelectricity exclusively due to changes between the ferroelastic domain population is elucidated as a function of epitaxial strain. Further, using highly sensitive thin-film resistive thermometry, direct electrocaloric temperature changes are measured on these polydomain thin films for the first time. The results demonstrate that temperature- and electric-field-driven domain interconversion under compressive strain diminish both the pyroelectric and the electrocaloric effects, while both these susceptibilities are enhanced due to the exact-opposite effect from the extrinsic contributions under tensile strain.},
doi = {10.1002/adma.201803312},
journal = {Advanced Materials},
number = 5,
volume = 31,
place = {United States},
year = {2018},
month = {12}
}

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Works referenced in this record:

Room-temperature ferroelectricity in strained SrTiO3
journal, August 2004

  • Haeni, J. H.; Irvin, P.; Chang, W.
  • Nature, Vol. 430, Issue 7001, p. 758-761
  • DOI: 10.1038/nature02773

Thermophysical properties of SrHfO3 and SrRuO3
journal, October 2004

  • Yamanaka, Shinsuke; Maekawa, Takuji; Muta, Hiroaki
  • Journal of Solid State Chemistry, Vol. 177, Issue 10
  • DOI: 10.1016/j.jssc.2004.05.039

Large Electrocaloric Effect in Ferroelectric Polymers Near Room Temperature
journal, August 2008


Effect of 90° Domain Walls on the Low-Field Permittivity of PbZr 0.2 Ti 0.8 O 3 Thin Films
journal, April 2012


Reduction of the electrocaloric entropy change of ferroelectric PbZr 1 x Ti x O 3 epitaxial layers due to an elastocaloric effect
journal, September 2014


Use of low‐frequency sinusoidal temperature waves to separate pyroelectric currents from nonpyroelectric currents. Part II. Experiment
journal, December 1982

  • Sharp, Edward J.; Garn, Lynn E.
  • Journal of Applied Physics, Vol. 53, Issue 12
  • DOI: 10.1063/1.330455

Caloric materials near ferroic phase transitions
journal, April 2014

  • Moya, X.; Kar-Narayan, S.; Mathur, N. D.
  • Nature Materials, Vol. 13, Issue 5
  • DOI: 10.1038/nmat3951

Highly mobile ferroelastic domain walls in compositionally graded ferroelectric thin films
journal, February 2016

  • Agar, J. C.; Damodaran, A. R.; Okatan, M. B.
  • Nature Materials, Vol. 15, Issue 5
  • DOI: 10.1038/nmat4567

A Strain-Driven Morphotropic Phase Boundary in BiFeO3
journal, November 2009

  • Zeches, R. J.; Rossell, M. D.; Zhang, J. X.
  • Science, Vol. 326, Issue 5955, p. 977-980
  • DOI: 10.1126/science.1177046

Quantitative and high spatial resolution d 33 measurement of piezoelectric bulk and thin films
journal, November 2015

  • Shetty, Smitha; Yang, Jung In; Stitt, Joe
  • Journal of Applied Physics, Vol. 118, Issue 17
  • DOI: 10.1063/1.4935140

Pyroelectric properties of polydomain epitaxial Pb ( Zr 1 x , Ti x ) O 3 thin films
journal, July 2011


Use of low‐frequency sinusoidal temperature waves to separate pyroelectric currents from nonpyroelectric currents. Part I. Theory
journal, December 1982

  • Garn, Lynn E.; Sharp, Edward J.
  • Journal of Applied Physics, Vol. 53, Issue 12
  • DOI: 10.1063/1.330454

Three-State Ferroelastic Switching and Large Electromechanical Responses in PbTiO 3 Thin Films
journal, July 2017

  • Damodaran, Anoop R.; Pandya, Shishir; Agar, Josh C.
  • Advanced Materials, Vol. 29, Issue 37
  • DOI: 10.1002/adma.201702069

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

Effect of domain walls on the electrocaloric properties of Pb(Zr 1−x ,Ti x )O 3 thin films
journal, July 2011

  • Karthik, J.; Martin, L. W.
  • Applied Physics Letters, Vol. 99, Issue 3
  • DOI: 10.1063/1.3614453

Pyroelectric conversion cycles
journal, December 1985

  • Olsen, Randall B.; Bruno, David A.; Briscoe, J. Merv
  • Journal of Applied Physics, Vol. 58, Issue 12
  • DOI: 10.1063/1.336244

Pyroelectric energy conversion with large energy and power density in relaxor ferroelectric thin films
journal, April 2018


Phase transitions of self-polarized PZT thin films
journal, January 2002

  • Suchaneck, Gunnar; Gerlach, Gerald; Deyneka, Alexander
  • MRS Proceedings, Vol. 718
  • DOI: 10.1557/PROC-718-D8.4

Specific heat and thermal conductivity of low-stress amorphous Si–N membranes
journal, January 2004


Advances in the growth and characterization of magnetic, ferroelectric, and multiferroic oxide thin films
journal, May 2010

  • Martin, L. W.; Chu, Y. -H.; Ramesh, R.
  • Materials Science and Engineering: R: Reports, Vol. 68, Issue 4-6
  • DOI: 10.1016/j.mser.2010.03.001

Strain on ferroelectric thin films: Example of Pb(Zr1−xTix)O3
journal, October 2009


Dielectric and pyroelectric properties in the Pb(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 system
journal, December 1989


Effect of 90° Domain Walls and Thermal Expansion Mismatch on the Pyroelectric Properties of Epitaxial PbZr 0.2 Ti 0.8 O 3 Thin Films
journal, December 2012


Growth and Investigation of Nd_{1-x}Sm_{x}ScO_3 and Sm_{1-x}Gd_{x}ScO_3 Solid-Solution Single Crystals
journal, August 2013


Phase-field modeling of the influence of domain structures on the electrocaloric effects in PbTiO3 thin films
journal, November 2014


Thermodynamic theory of epitaxial ferroelectric thin films with dense domain structures
journal, November 2001


Direct Measurement of Pyroelectric and Electrocaloric Effects in Thin Films
journal, March 2017


Highly efficient electrocaloric cooling with electrostatic actuation
journal, September 2017


Invited Review Article: Practical guide for pyroelectric measurements
journal, May 2012

  • Lubomirsky, Igor; Stafsudd, Oscar
  • Review of Scientific Instruments, Vol. 83, Issue 5
  • DOI: 10.1063/1.4709621

Electrocaloric enhancement near the morphotropic phase boundary in lead-free NBT-KBT ceramics
journal, October 2015

  • Le Goupil, Florian; Bennett, James; Axelsson, Anna-Karin
  • Applied Physics Letters, Vol. 107, Issue 17
  • DOI: 10.1063/1.4934759

Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics
journal, May 2017

  • Damodaran, Anoop R.; Pandya, Shishir; Qi, Yubo
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14961

Relative coherency strain and phase transformation history in epitaxial ferroelectric thin films
journal, February 1996

  • Foster, C. M.; Pompe, W.; Daykin, A. C.
  • Journal of Applied Physics, Vol. 79, Issue 3
  • DOI: 10.1063/1.360978

Giant Electrocaloric Strength in Single-Crystal BaTiO 3
journal, January 2013

  • Moya, Xavier; Stern-Taulats, Enric; Crossley, Sam
  • Advanced Materials, Vol. 25, Issue 9
  • DOI: 10.1002/adma.201203823

High-pressure synthesis of the cubic perovskite BaRuO3 and evolution of ferromagnetism in ARuO3 (A = Ca, Sr, Ba) ruthenates
journal, May 2008

  • Jin, C. -Q.; Zhou, J. -S.; Goodenough, J. B.
  • Proceedings of the National Academy of Sciences, Vol. 105, Issue 20
  • DOI: 10.1073/pnas.0710928105

Pyroelectric devices and materials
journal, December 1986


Domain wall motion and its contribution to the dielectric and piezoelectric properties of lead zirconate titanate films
journal, January 2001

  • Xu, F.; Trolier-McKinstry, S.; Ren, W.
  • Journal of Applied Physics, Vol. 89, Issue 2
  • DOI: 10.1063/1.1325005

Enhancement of Ferroelectricity in Strained BaTiO3 Thin Films
journal, November 2004


Pyroelectric thin-film sensor array
journal, May 1997


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


The elastic, piezoelectric and dielectric constants of tetragonal PbTiO3 single crystals
journal, March 1993


Large electrocaloric effect induced by the multi-domain to mono-domain transition in ferroelectrics
journal, April 2014

  • Wang, Jie; Liu, Man; Zhang, Yajun
  • Journal of Applied Physics, Vol. 115, Issue 16
  • DOI: 10.1063/1.4873112

Electrocaloric Materials for Solid-State Refrigeration
journal, May 2009

  • Lu, Sheng-Guo; Zhang, Qiming
  • Advanced Materials, Vol. 21, Issue 19, p. 1983-1987
  • DOI: 10.1002/adma.200802902

Strain Tuning of Ferroelectric Thin Films
journal, August 2007


    Works referencing / citing this record:

    Large Polarization and Susceptibilities in Artificial Morphotropic Phase Boundary PbZr 1− x Ti x O 3 Superlattices
    journal, January 2020

    • Lupi, Eduardo; Ghosh, Anirban; Saremi, Sahar
    • Advanced Electronic Materials, Vol. 6, Issue 3
    • DOI: 10.1002/aelm.201901395

    New approach to waste-heat energy harvesting: pyroelectric energy conversion
    journal, June 2019


    Ferroelectric domain structures and temperature-misfit strain phase diagrams of K 1-x Na x NbO 3 thin films: A phase-field study
    journal, August 2019

    • Wang, Bo; Chen, Hao-Nan; Wang, Jian-Jun
    • Applied Physics Letters, Vol. 115, Issue 9
    • DOI: 10.1063/1.5116910

    Enhanced pyroelectric properties of Bi 1−x La x FeO 3 thin films
    journal, November 2019

    • Zhang, Lei; Huang, Yen-Lin; Velarde, Gabriel
    • APL Materials, Vol. 7, Issue 11
    • DOI: 10.1063/1.5128413

    Analytical description of the size effect on pyroelectric and electrocaloric properties of ferroelectric nanoparticles
    journal, October 2019