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Title: Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics

A range of modern applications require large and tunable dielectric, piezoelectric or pyroelectric response of ferroelectrics. Such effects are intimately connected to the nature of polarization and how it responds to externally applied stimuli. Ferroelectric susceptibilities are, in general, strongly temperature dependent, diminishing rapidly as one transitions away from the ferroelectric phase transition (T C). In turn, researchers seek new routes to manipulate polarization to simultaneously enhance susceptibilities and broaden operational temperature ranges. Here, we demonstrate such a capability by creating composition and strain gradients in Ba 1-xSr xTiO 3 films which result in spatial polarization gradients as large as 35 μC cm -2 across a 150 nm thick film. These polarization gradients allow for large dielectric permittivity with low loss (ε r≈775, tan δ<0.05), negligible temperature-dependence (13% deviation over 500 °C) and high-dielectric tunability (greater than 70% across a 300 °C range). The role of space charges in stabilizing polarization gradients is also discussed.
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [1] ; ORCiD logo [3] ;  [4] ;  [1] ; ORCiD logo [5] ;  [5] ;  [1] ;  [1] ;  [1] ;  [6] ;  [4] ; ORCiD logo [2] ; ORCiD logo [7]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
  3. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry; Carnegie Inst. for Science, Washington, DC (United States). Geophysical Lab.
  4. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy
  6. Rutgers Univ., Piscataway, NJ (United States). Dept. of Physics and Astronomy
  7. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Publication Date:
Grant/Contract Number:
AC02-05CH11231; SC0012375; CMMI-1334241; DMR-1451219; CMMI-1434147; DMR-1608938
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (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:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; ferroelectronics and multiferroics; phase transitions and critical phenomena
OSTI Identifier:
1379845

Damodaran, Anoop R., Pandya, Shishir, Qi, Yubo, Hsu, Shang-Lin, Liu, Shi, Nelson, Christopher, Dasgupta, Arvind, Ercius, Peter, Ophus, Colin, Dedon, Liv R., Agar, Josh C., Lu, Hongling, Zhang, Jialan, Minor, Andrew M., Rappe, Andrew M., and Martin, Lane W.. Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics. United States: N. p., Web. doi:10.1038/ncomms14961.
Damodaran, Anoop R., Pandya, Shishir, Qi, Yubo, Hsu, Shang-Lin, Liu, Shi, Nelson, Christopher, Dasgupta, Arvind, Ercius, Peter, Ophus, Colin, Dedon, Liv R., Agar, Josh C., Lu, Hongling, Zhang, Jialan, Minor, Andrew M., Rappe, Andrew M., & Martin, Lane W.. Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics. United States. doi:10.1038/ncomms14961.
Damodaran, Anoop R., Pandya, Shishir, Qi, Yubo, Hsu, Shang-Lin, Liu, Shi, Nelson, Christopher, Dasgupta, Arvind, Ercius, Peter, Ophus, Colin, Dedon, Liv R., Agar, Josh C., Lu, Hongling, Zhang, Jialan, Minor, Andrew M., Rappe, Andrew M., and Martin, Lane W.. 2017. "Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics". United States. doi:10.1038/ncomms14961. https://www.osti.gov/servlets/purl/1379845.
@article{osti_1379845,
title = {Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics},
author = {Damodaran, Anoop R. and Pandya, Shishir and Qi, Yubo and Hsu, Shang-Lin and Liu, Shi and Nelson, Christopher and Dasgupta, Arvind and Ercius, Peter and Ophus, Colin and Dedon, Liv R. and Agar, Josh C. and Lu, Hongling and Zhang, Jialan and Minor, Andrew M. and Rappe, Andrew M. and Martin, Lane W.},
abstractNote = {A range of modern applications require large and tunable dielectric, piezoelectric or pyroelectric response of ferroelectrics. Such effects are intimately connected to the nature of polarization and how it responds to externally applied stimuli. Ferroelectric susceptibilities are, in general, strongly temperature dependent, diminishing rapidly as one transitions away from the ferroelectric phase transition (TC). In turn, researchers seek new routes to manipulate polarization to simultaneously enhance susceptibilities and broaden operational temperature ranges. Here, we demonstrate such a capability by creating composition and strain gradients in Ba1-xSrxTiO3 films which result in spatial polarization gradients as large as 35 μC cm-2 across a 150 nm thick film. These polarization gradients allow for large dielectric permittivity with low loss (εr≈775, tan δ<0.05), negligible temperature-dependence (13% deviation over 500 °C) and high-dielectric tunability (greater than 70% across a 300 °C range). The role of space charges in stabilizing polarization gradients is also discussed.},
doi = {10.1038/ncomms14961},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}