Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control
Abstract
The desire for low-power/voltage operation of devices is driving renewed interest in understanding scaling effects in ferroelectric thin films. As the dimensions of ferroelectrics are reduced, the properties can vary dramatically, including the robust scaling relationship between coercive field (Ec) and thickness (d), also referred to as the Janovec-Kay-Dunn (JKD) law, wherein Ec ∝ d-2/3. Here, we report that whereas (001)-oriented heterostructures follow JKD scaling across the thicknesses range of 20-330 nm, (111)-oriented heterostructures of the canonical tetragonal ferroelectric PbZr0.2Ti0.8O3 exhibit a deviation from JKD scaling wherein a smaller scaling exponent for the evolution of Ec is observed in films of thickness ≤ 165 nm. X-ray diffraction reveals that whereas (001)-oriented heterostructures remain tetragonal for all thicknesses, (111)-oriented heterostructures exhibit a transition from tetragonal-to-monoclinic symmetry in films of thickness ≤ 165 nm as a result of the compressive strain. First-principles calculations suggest that this symmetry change contributes to the deviation from the expected scaling, as the monoclinic phase has a lower energy barrier for switching. This structural evolution also gives rise to changes in the c/a lattice parameter ratio, wherein this ratio increases and decreases in (001)- and (111)-oriented heterostructures, respectively, as the films are made thinner. In (111)-oriented heterostructures,more »
- Authors:
-
- Univ. of California, Berkeley, CA (United States)
- Univ. Andres Bello, Santiago (Chile); Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of Science and Technology of China, Hefei (China)
- Harbin Institute of Technology, Harbin (China)
- Hubei Univ., Wuhan (China)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute at Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1466327
- Alternate Identifier(s):
- OSTI ID: 1462002
- Grant/Contract Number:
- AC02-06CH11357; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 5; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; coercive-field scaling; ferroelectric; size effects; thin film; x-ray diffraction
Citation Formats
Xu, Ruijuan, Gao, Ran, Reyes-Lillo, Sebastian E., Saremi, Sahar, Dong, Yongqi, Lu, Hongling, Chen, Zuhuang, Lu, Xiaoyan, Qi, Yajun, Hsu, Shang-Lin, Damodaran, Anoop R., Zhou, Hua, Neaton, Jeffrey B., and Martin, Lane W. Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control. United States: N. p., 2018.
Web. doi:10.1021/acsnano.8b01399.
Xu, Ruijuan, Gao, Ran, Reyes-Lillo, Sebastian E., Saremi, Sahar, Dong, Yongqi, Lu, Hongling, Chen, Zuhuang, Lu, Xiaoyan, Qi, Yajun, Hsu, Shang-Lin, Damodaran, Anoop R., Zhou, Hua, Neaton, Jeffrey B., & Martin, Lane W. Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control. United States. https://doi.org/10.1021/acsnano.8b01399
Xu, Ruijuan, Gao, Ran, Reyes-Lillo, Sebastian E., Saremi, Sahar, Dong, Yongqi, Lu, Hongling, Chen, Zuhuang, Lu, Xiaoyan, Qi, Yajun, Hsu, Shang-Lin, Damodaran, Anoop R., Zhou, Hua, Neaton, Jeffrey B., and Martin, Lane W. Wed .
"Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control". United States. https://doi.org/10.1021/acsnano.8b01399. https://www.osti.gov/servlets/purl/1466327.
@article{osti_1466327,
title = {Reducing Coercive-Field Scaling in Ferroelectric Thin Films via Orientation Control},
author = {Xu, Ruijuan and Gao, Ran and Reyes-Lillo, Sebastian E. and Saremi, Sahar and Dong, Yongqi and Lu, Hongling and Chen, Zuhuang and Lu, Xiaoyan and Qi, Yajun and Hsu, Shang-Lin and Damodaran, Anoop R. and Zhou, Hua and Neaton, Jeffrey B. and Martin, Lane W.},
abstractNote = {The desire for low-power/voltage operation of devices is driving renewed interest in understanding scaling effects in ferroelectric thin films. As the dimensions of ferroelectrics are reduced, the properties can vary dramatically, including the robust scaling relationship between coercive field (Ec) and thickness (d), also referred to as the Janovec-Kay-Dunn (JKD) law, wherein Ec ∝ d-2/3. Here, we report that whereas (001)-oriented heterostructures follow JKD scaling across the thicknesses range of 20-330 nm, (111)-oriented heterostructures of the canonical tetragonal ferroelectric PbZr0.2Ti0.8O3 exhibit a deviation from JKD scaling wherein a smaller scaling exponent for the evolution of Ec is observed in films of thickness ≤ 165 nm. X-ray diffraction reveals that whereas (001)-oriented heterostructures remain tetragonal for all thicknesses, (111)-oriented heterostructures exhibit a transition from tetragonal-to-monoclinic symmetry in films of thickness ≤ 165 nm as a result of the compressive strain. First-principles calculations suggest that this symmetry change contributes to the deviation from the expected scaling, as the monoclinic phase has a lower energy barrier for switching. This structural evolution also gives rise to changes in the c/a lattice parameter ratio, wherein this ratio increases and decreases in (001)- and (111)-oriented heterostructures, respectively, as the films are made thinner. In (111)-oriented heterostructures, this reduced tetragonality drives a reduction of the remanent polarization and, therefore, a reduction of the domain-wall energy and overall energy barrier to switching, which further exacerbates the deviation from the expected scaling. Altogether, this work demonstrates a route toward reducing coercive fields in ferroelectric thin films and provides a possible mechanism to understand the deviation from JKD scaling.},
doi = {10.1021/acsnano.8b01399},
journal = {ACS Nano},
number = 5,
volume = 12,
place = {United States},
year = {Wed Apr 11 00:00:00 EDT 2018},
month = {Wed Apr 11 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Ferroelectric thin films: Review of materials, properties, and applications
journal, September 2006
- Setter, N.; Damjanovic, D.; Eng, L.
- Journal of Applied Physics, Vol. 100, Issue 5
Applications of Modern Ferroelectrics
journal, February 2007
- Scott, J. F.
- Science, Vol. 315, Issue 5814
Complementary ferroelectric-capacitor logic for low-power logic-in-memory VLSI
journal, June 2004
- Kimura, H.; Hanyu, T.; Kameyama, M.
- IEEE Journal of Solid-State Circuits, Vol. 39, Issue 6
A diode for ferroelectric domain-wall motion
journal, June 2015
- Whyte, J. R.; Gregg, J. M.
- Nature Communications, Vol. 6, Issue 1
Ferroelectric thin film technology for semiconductor memory
journal, April 1995
- Moazzami, R.
- Semiconductor Science and Technology, Vol. 10, Issue 4
Regular arrays of highly ordered ferroelectric polymer nanostructures for non-volatile low-voltage memories
journal, December 2008
- Hu, Zhijun; Tian, Mingwen; Nysten, Bernard
- Nature Materials, Vol. 8, Issue 1
Scaling Effects in Perovskite Ferroelectrics: Fundamental Limits and Process-Structure-Property Relations
journal, July 2016
- Ihlefeld, Jon F.; Harris, David T.; Keech, Ryan
- Journal of the American Ceramic Society, Vol. 99, Issue 8
Scaling of structure and electrical properties in ultrathin epitaxial ferroelectric heterostructures
journal, September 2006
- Nagarajan, V.; Junquera, J.; He, J. Q.
- Journal of Applied Physics, Vol. 100, Issue 5
Thickness-dependent evolutions of domain configuration and size in ferroelectric and ferroelectric-ferroelastic films
journal, March 2013
- Huang, C. W.; Chen, Z. H.; Chen, Lang
- Journal of Applied Physics, Vol. 113, Issue 9
Suppressed Dependence of Polarization on Epitaxial Strain in Highly Polar Ferroelectrics
journal, May 2007
- Lee, Ho Nyung; Nakhmanson, Serge M.; Chisholm, Matthew F.
- Physical Review Letters, Vol. 98, Issue 21
Ferroelectricity in Ultrathin Perovskite Films
journal, June 2004
- Fong, Dillon D.; Stephenson, G. Brian; Streiffer, Stephen K.
- Science, Vol. 304, Issue 5677, p. 1650-1653
Coercive field of ultrathin Pb(Zr0.52Ti0.48)O3 epitaxial films
journal, October 2003
- Pertsev, N. A.; Rodrı́guez Contreras, J.; Kukhar, V. G.
- Applied Physics Letters, Vol. 83, Issue 16
Mechanism of Fatigue in Ferroelectric Thin Films
journal, October 1992
- Yoo, I. K.; Desu, S. B.
- Physica Status Solidi (a), Vol. 133, Issue 2
Identification of passive layer in ferroelectric thin films from their switching parameters
journal, August 1995
- Tagantsev, A. K.; Landivar, M.; Colla, E.
- Journal of Applied Physics, Vol. 78, Issue 4
Ferroelectric properties and fatigue of PbZr 0.51 Ti 0.49 O 3 thin films of varying thickness: Blocking layer model
journal, August 1994
- Larsen, P. K.; Dormans, G. J. M.; Taylor, D. J.
- Journal of Applied Physics, Vol. 76, Issue 4
Advanced synthesis techniques and routes to new single-phase multiferroics
journal, October 2012
- Martin, Lane W.; Schlom, Darrell G.
- Current Opinion in Solid State and Materials Science, Vol. 16, Issue 5
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
On the theory of the coercive field of single-domain crystals of BaTiO3
journal, January 1958
- Janovec, Václav
- Czechoslovak Journal of Physics, Vol. 8, Issue 1
Thickness dependence of the nucleation field of triglycine sulphate
journal, December 1962
- Kay, H. F.; Dunn, J. W.
- Philosophical Magazine, Vol. 7, Issue 84
Scaling of the Coercive Field with Thickness in Thin-Film Ferroelectrics
journal, January 2004
- Chandra, P.; Dawber, M.; Littlewood, P. B.
- Ferroelectrics, Vol. 313, Issue 1
Two-dimensional ferroelectric films
journal, February 1998
- Bune, A. V.; Fridkin, V. M.; Ducharme, Stephen
- Nature, Vol. 391, Issue 6670, p. 874-877
Intrinsic Ferroelectric Coercive Field
journal, January 2000
- Ducharme, Stephen; Fridkin, V. M.; Bune, A. V.
- Physical Review Letters, Vol. 84, Issue 1
Coercive fields in ultrathin BaTiO3 capacitors
journal, December 2006
- Jo, J. Y.; Kim, Y. S.; Noh, T. W.
- Applied Physics Letters, Vol. 89, Issue 23
Depolarization corrections to the coercive field in thin-film ferroelectrics
journal, June 2003
- Dawber, M.; Chandra, P.; Littlewood, P. B.
- Journal of Physics: Condensed Matter, Vol. 15, Issue 24
Stationary domain wall contribution to enhanced ferroelectric susceptibility
journal, January 2014
- Xu, Ruijuan; Karthik, J.; Damodaran, Anoop R.
- Nature Communications, Vol. 5, Issue 1
Ferroelectric polarization reversal via successive ferroelastic transitions
journal, October 2014
- Xu, Ruijuan; Liu, Shi; Grinberg, Ilya
- Nature Materials, Vol. 14, Issue 1
Thickness dependence of polarization in ferroelectric perovskite thin films
journal, February 2005
- Liu, Gang; Nan, Ce-Wen
- Journal of Physics D: Applied Physics, Vol. 38, Issue 4
Intrinsic ferroelectric switching from first principles
journal, June 2016
- Liu, Shi; Grinberg, Ilya; Rappe, Andrew M.
- Nature, Vol. 534, Issue 7607
Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981
- Perdew, J. P.; Zunger, Alex
- Physical Review B, Vol. 23, Issue 10, p. 5048-5079
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Effect of Mechanical Boundary Conditions on Phase Diagrams of Epitaxial Ferroelectric Thin Films
journal, March 1998
- Pertsev, N. A.; Zembilgotov, A. G.; Tagantsev, A. K.
- Physical Review Letters, Vol. 80, Issue 9
First-principles study of epitaxial strain in perovskites
journal, October 2005
- Diéguez, Oswaldo; Rabe, Karin M.; Vanderbilt, David
- Physical Review B, Vol. 72, Issue 14
Strain-induced diffuse dielectric anomaly and critical point in perovskite ferroelectric thin films
journal, December 2001
- Tagantsev, A. K.; Pertsev, N. A.; Muralt, P.
- Physical Review B, Vol. 65, Issue 1
Computational study of (111) epitaxially strained ferroelectric perovskites and
journal, September 2008
- Oja, Riku; Johnston, Karen; Frantti, Johannes
- Physical Review B, Vol. 78, Issue 9
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Theory of polarization of crystalline solids
journal, January 1993
- King-Smith, R. D.; Vanderbilt, David
- Physical Review B, Vol. 47, Issue 3
Works referencing / citing this record:
Obvious ferroelectricity in undoped HfO 2 films by chemical solution deposition
journal, January 2020
- Chen, Haiyan; Chen, Yonghong; Tang, Lin
- Journal of Materials Chemistry C, Vol. 8, Issue 8
Progress, Outlook, and Challenges in Lead‐Free Energy‐Storage Ferroelectrics
journal, December 2019
- Sun, Zixiong; Wang, Zhuo; Tian, Ye
- Advanced Electronic Materials, Vol. 6, Issue 1