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

doi:10.1038/ncomms14961

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 journal › Article › peer-review

62 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 (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_xTiO₃ 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 language	English
Article number	14961
Journal	Nature Communications
Volume	8
DOIs	https://doi.org/10.1038/ncomms14961
State	Published - 2017
Externally published	Yes

Funding

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. 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.

Funders	Funder number
Office of Basic Science
National Science Foundation	CMMI-1334241
Office of Naval Research	DMR-1608938, N00014-12-1-1033
U.S. Department of Energy	DE-AC02-05CH11231, DE-SC0012375
Army Research Office	W911NF-14-1-0104
Gordon and Betty Moore Foundation	GBMF5307
Carnegie Institution of Washington
Office of Science
Basic Energy Sciences	DE-FG02-07ER15920
Materials Research Science and Engineering Center, Harvard University	DMR-1420620
National Science Foundation	DMR-1451219, CMMI-1434147

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Damodaran, A. R., Pandya, S., Qi, Y., Hsu, S. L., Liu, S., Nelson, C., Dasgupta, A., Ercius, P., Ophus, C., Dedon, L. R., Agar, J. C., Lu, H., Zhang, J., Andrew, M., Rappe, A. M., & Martin, L. W. (2017). Large polarization gradients and temperature-stable responses in compositionally-graded ferroelectrics. Nature Communications, 8, Article 14961. https://doi.org/10.1038/ncomms14961

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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.",

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AU - Hsu, Shang Lin

AU - Liu, Shi

AU - Nelson, Christopher

AU - Dasgupta, Arvind

AU - Ercius, Peter

AU - Ophus, Colin

AU - Dedon, Liv R.

AU - Agar, Josh C.

AU - Lu, Hongling

AU - Zhang, Jialan

AU - Andrew, Minor

AU - Rappe, Andrew M.

AU - Martin, Lane W.

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

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