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

Anoop R. Damodaran, Shishir Pandya, Yubo Qi, Shang Lin Hsu, Shi Liu, Christopher Nelson, Arvind Dasgupta, Peter Ercius, Colin Ophus, Liv R. Dedon, Josh C. Agar, Hongling Lu, Jialan Zhang, Minor Andrew, Andrew M. Rappe, Lane W. Martin

Research output: Contribution to journalArticlepeer-review

33 Scopus citations

Abstract

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 35μCcm-2 across a 150nm thick film. These polarization gradients allow for large dielectric permittivity with low loss (er≈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.

Original languageEnglish (US)
Article number14961
JournalNature communications
Volume8
DOIs
StatePublished - 2017
Externally publishedYes

Bibliographical note

Funding Information:
We acknowledge I. Grinberg for fruitful discussions and help in understanding these results. A.R.D. and S.P. acknowledge support from the Army Research Office under grant W911NF-14-1-0104. Y.Q. acknowledges support from the National Science Foundation under grant CMMI-1334241. S.L.H. acknowledges support from National Science Foundation under MRSEC programme DMR-1420620. S.L. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, under grant DE-FG02-07ER15920, as well as support from the Carnegie Institution for Science. C.T.N. acknowledges support from Office of Basic Science, of the U.S. Department of Energy, under Contract No. DE-AC02-05CH11231. A.D. acknowledges support from the Department of Energy under grant DE-SC0012375 for synthesis of the materials. L.D. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF5307. J.C.A. and H.L. acknowledge support from the National Science Foundation under grant DMR-1451219. J.Z. acknowledges support from the National Science Foundation under grant CMMI-1434147. A.M.R. acknowledges support from the Office of Naval Research, under grant N00014-12-1-1033. L.W.M. acknowledges support from the National Science Foundation under grant DMR-1608938. The authors also acknowledge computational support from the HPCMO of the DoD and the NERSC of the DoE. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Funding Information:
We acknowledge I. Grinberg for fruitful discussions and help in understanding these results. A.R.D. and S.P. acknowledge support from the Army Research Office under grant W911NF-14-1-0104. Y.Q. acknowledges support from the National Science Foundation under grant CMMI-1334241. S.L.H. acknowledges support from National Science Foundation under MRSEC programme DMR-1420620. S.L. acknowledges support from the US Department of Energy, Office of Basic Energy Sciences, under grant DE-FG02-07ER15920, as well as support from the Carnegie Institution for Science. C.T.N. acknowledges support from Office of Basic Science, of the U.S. Department of Energy, under Contract No. DE-AC02-05CH11231. A.D. acknowledges support from the Department of Energy under grant DE-SC0012375 for synthesis of the materials. L.D. acknowledges support from the Gordon and Betty Moore Foundation's EPiQS Initiative, Grant GBMF5307. J.C.A. and H.L. acknowledge support from the National Science Foundation under grant DMR-1451219. J.Z. acknowledges support from the National Science Foundation under grant CMMI-1434147. A.M.R. acknowledges support from the Office of Naval Research, under grant N00014-12-1-1033. L.W.M. acknowledges support from the National Science Foundation under grant DMR-1608938. The authors also acknowledge computational support from the HPCMO of the DoD and the NERSC of the DoE. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Publisher Copyright:
© The Author(s) 2017.

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