Anisotropic epitaxial stabilization of a low-symmetry ferroelectric with enhanced electromechanical response

Paull, Oliver; Xu, Changsong; Cheng, Xuan; Zhang, Yangyang; Xu, Bin; Kelley, Kyle P.; de Marco, Alex; Vasudevan, Rama K.; Bellaiche, Laurent; Nagarajan, Valanoor; Sando, Daniel

doi:10.1038/s41563-021-01098-w

Anisotropic epitaxial stabilization of a low-symmetry ferroelectric with enhanced electromechanical response

Journal Article · Thu Sep 23 00:00:00 EDT 2021 · Nature Materials

DOI:https://doi.org/10.1038/s41563-021-01098-w· OSTI ID:1844910

Paull, Oliver ^[1]; Xu, Changsong ^[2]; Cheng, Xuan ^[3]; Zhang, Yangyang ^[1]; ^[4]; ^[5]; de Marco, Alex ^[3]; ^[5]; ^[2]; ^[1]; ^[1]

Univ. of New South Wales, Sydney, NSW (Australia)
Univ. of Arkansas, Fayetteville, AR (United States)
Monash Univ., Melbourne, VIC (Australia)
Univ. of Arkansas, Fayetteville, AR (United States); Soochow University, Suzhou (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Here piezoelectrics interconvert mechanical energy and electric charge and are widely used in actuators and sensors. The best performing materials are ferroelectrics at a morphotropic phase boundary, where several phases coexist. Switching between these phases by electric field produces a large electromechanical response. In ferroelectric BiFeO3, strain can create a morphotropic-phase-boundary-like phase mixture and thus generate large electric-field-dependent strains. However, this enhanced response occurs at localized, randomly positioned regions of the film. Here, we use epitaxial strain and orientation engineering in tandem-anisotropic epitaxy-to craft a low-symmetry phase of BiFeO3 that acts as a structural bridge between the rhombohedral-like and tetragonal-like polymorphs. Interferometric displacement sensor measurements reveal that this phase has an enhanced piezoelectric coefficient of x2.4 compared with typical rhombohedral-like BiFeO3. Band-excitation frequency response measurements and first-principles calculations provide evidence that this phase undergoes a transition to the tetragonal-like polymorph under electric field, generating an enhanced piezoelectric response throughout the film and associated field-induced reversible strains. These results offer a route to engineer thin-film piezoelectrics with improved functionalities, with broader perspectives for other functional oxides.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Australian Research Council (ARC); Defense Advanced Research Projects Agency (DARPA); National Natural Science Foundation of China; Natural Science Foundation of Jiangsu Province; USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1844910

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 1 Vol. 21; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (58)

Novel Nanoscale Twinned Phases in Perovskite Oxides Prosandeev, Sergey; Wang, Dawei; Ren, Wei Advanced Functional Materials, Vol. 23, Issue 2 https://doi.org/10.1002/adfm.201201467	journal	August 2012
Nanoscale Structure and Mechanism for Enhanced Electromechanical Response of Highly Strained BiFeO₃ Thin Films Damodaran, Anoop R.; Liang, Chen-Wei; He, Qing Advanced Materials, Vol. 23, Issue 28, p. 3170-3175 https://doi.org/10.1002/adma.201101164	journal	May 2011
Nanoscale Mechanical Softening of Morphotropic BiFeO ₃ Heo, Yooun; Jang, Byong-Kweon; Kim, Seung Jin Advanced Materials, Vol. 26, Issue 45 https://doi.org/10.1002/adma.201401958	journal	October 2014
Positive Effect of an Internal Depolarization Field in Ultrathin Epitaxial Ferroelectric Films Liu, Guangqing; Chen, Jason; Lichtensteiger, Céline Advanced Electronic Materials, Vol. 2, Issue 1 https://doi.org/10.1002/aelm.201500288	journal	November 2015
Manufacture of Piezoelectric Ceramics Jaffe, Bernard; Cook, Jr., William Rjj.; Jaffe, Hans Piezoelectric Ceramics, p. 253-269 https://doi.org/10.1016/B978-0-12-379550-2.50015-6	book	January 1971
Quantitative measurement of displacement and strain fields from HREM micrographs Hÿtch, M. J.; Snoeck, E.; Kilaas, R. Ultramicroscopy, Vol. 74, Issue 3, p. 131-146 https://doi.org/10.1016/S0304-3991(98)00035-7	journal	August 1998
Advantages and challenges of relaxor-PbTiO3 ferroelectric crystals for electroacoustic transducers – A review Zhang, Shujun; Li, Fei; Jiang, Xiaoning Progress in Materials Science, Vol. 68 https://doi.org/10.1016/j.pmatsci.2014.10.002	journal	March 2015
Probing Local Bias-Induced Transitions Using Photothermal Excitation Contact Resonance Atomic Force Microscopy and Voltage Spectroscopy Li, Qian; Jesse, Stephen; Tselev, Alexander ACS Nano, Vol. 9, Issue 2 https://doi.org/10.1021/nn506753u	journal	January 2015
Polarization rotation mechanism for ultrahigh electromechanical response in single-crystal piezoelectrics Fu, Huaxiang; Cohen, Ronald E. Nature, Vol. 403, Issue 6767 https://doi.org/10.1038/35002022	journal	January 2000
Lead-free piezoceramics Saito, Yasuyoshi; Takao, Hisaaki; Tani, Toshihiko Nature, Vol. 432, Issue 7013 https://doi.org/10.1038/nature03028	journal	October 2004
Materials science: Lead-free at last Cross, Eric Nature, Vol. 432, Issue 7013, p. 24-25 https://doi.org/10.1038/nature03142	journal	October 2004
Origin of morphotropic phase boundaries in ferroelectrics Ahart, Muhtar; Somayazulu, Maddury; Cohen, R. E. Nature, Vol. 451, Issue 7178 https://doi.org/10.1038/nature06459	journal	January 2008
Large elasto-optic effect and reversible electrochromism in multiferroic BiFeO3 Sando, D.; Yang, Yurong; Bousquet, E. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10718	journal	February 2016
Atomic-scale evolution of modulated phases at the ferroelectric–antiferroelectric morphotropic phase boundary controlled by flexoelectric interaction Borisevich, A. Y.; Eliseev, E. A.; Morozovska, A. N. Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1778	journal	January 2012
Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching Ren, Xiaobing Nature Materials, Vol. 3, Issue 2 https://doi.org/10.1038/nmat1051	journal	January 2004
Ferroelastic switching for nanoscale non-volatile magnetoelectric devices Baek, S. H.; Jang, H. W.; Folkman, C. M. Nature Materials, Vol. 9, Issue 4 https://doi.org/10.1038/nmat2703	journal	February 2010
Crafting the magnonic and spintronic response of BiFeO3 films by epitaxial strain Sando, D.; Agbelele, A.; Rahmedov, D. Nature Materials, Vol. 12, Issue 7 https://doi.org/10.1038/nmat3629	journal	April 2013
Ferroelectric polarization reversal via successive ferroelastic transitions Xu, Ruijuan; Liu, Shi; Grinberg, Ilya Nature Materials, Vol. 14, Issue 1 https://doi.org/10.1038/nmat4119	journal	October 2014
Large field-induced strains in a lead-free piezoelectric material Zhang, J. X.; Xiang, B.; He, Q. Nature Nanotechnology, Vol. 6, Issue 2, p. 98-102 https://doi.org/10.1038/nnano.2010.265	journal	January 2011
An integrated optical modulator operating at cryogenic temperatures Eltes, Felix; Villarreal-Garcia, Gerardo E.; Caimi, Daniele Nature Materials, Vol. 19, Issue 11 https://doi.org/10.1038/s41563-020-0725-5	journal	July 2020
A monoclinic ferroelectric phase in the Pb(Zr1−xTix)O3 solid solution Noheda, B.; Cox, D. E.; Shirane, G. Applied Physics Letters, Vol. 74, Issue 14 https://doi.org/10.1063/1.123756	journal	April 1999
Rotator and extender ferroelectrics: Importance of the shear coefficient to the piezoelectric properties of domain-engineered crystals and ceramics Davis, Matthew; Budimir, Marko; Damjanovic, Dragan Journal of Applied Physics, Vol. 101, Issue 5 https://doi.org/10.1063/1.2653925	journal	March 2007
Origin of high piezoelectric response of Pb(ZrxTi1−x)O3 at the morphotropic phase boundary: Role of elastic instability Singh, Akhilesh Kumar; Mishra, Sunil Kumar Applied Physics Letters, Vol. 92, Issue 2 https://doi.org/10.1063/1.2836269	journal	January 2008
Ferroelectric solid solutions with morphotropic boundaries: Vanishing polarization anisotropy, adaptive, polar glass, and two-phase states Rossetti, G. A.; Khachaturyan, A. G.; Akcay, G. Journal of Applied Physics, Vol. 103, Issue 11 https://doi.org/10.1063/1.2930883	journal	June 2008
Triclinic phase in tilted (001) oriented BiFeO3 epitaxial thin films Yan, Li; Cao, Hu; Li, Jiefang Applied Physics Letters, Vol. 94, Issue 13 https://doi.org/10.1063/1.3110972	journal	March 2009
Quantitative measurements of electromechanical response with a combined optical beam and interferometric atomic force microscope Labuda, Aleksander; Proksch, Roger Applied Physics Letters, Vol. 106, Issue 25 https://doi.org/10.1063/1.4922210	journal	June 2015
A multiferroic on the brink: Uncovering the nuances of strain-induced transitions in BiFeO3 Sando, D.; Xu, Bin; Bellaiche, L. Applied Physics Reviews, Vol. 3, Issue 1 https://doi.org/10.1063/1.4944558	journal	March 2016
Band excitation in scanning probe microscopy: sines of change Jesse, Stephen; Kalinin, Sergei V. Journal of Physics D: Applied Physics, Vol. 44, Issue 46 https://doi.org/10.1088/0022-3727/44/46/464006	journal	November 2011
Strain dependence of polarization and piezoelectric response in epitaxial BiFeO ₃ thin films Daumont, C.; Ren, W.; Infante, I. C. Journal of Physics: Condensed Matter, Vol. 24, Issue 16 https://doi.org/10.1088/0953-8984/24/16/162202	journal	March 2012
Theory of polarization of crystalline solids King-Smith, R. D.; Vanderbilt, David Physical Review B, Vol. 47, Issue 3 https://doi.org/10.1103/PhysRevB.47.1651	journal	January 1993
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Stability of the monoclinic phase in the ferroelectric perovskite PbZr 1 − x Ti x O 3 Noheda, B.; Cox, D. E.; Shirane, G. Physical Review B, Vol. 63, Issue 1 https://doi.org/10.1103/PhysRevB.63.014103	journal	December 2000
Nanodomain structure of Pb [ Zr 1 − x Ti x ] O 3 at its morphotropic phase boundary: Investigations from local to average structure Schönau, Kristin A.; Schmitt, Ljubomira A.; Knapp, Michael Physical Review B, Vol. 75, Issue 18 https://doi.org/10.1103/PhysRevB.75.184117	journal	May 2007
Elastic properties of cubic and rhombohedral BiFeO 3 from first-principles calculations Shang, S. L.; Sheng, G.; Wang, Y. Physical Review B, Vol. 80, Issue 5 https://doi.org/10.1103/PhysRevB.80.052102	journal	August 2009
Coexistence of ferroelectric triclinic phases in highly strained BiFeO 3 films Chen, Zuhuang; Prosandeev, S.; Luo, Z. L. Physical Review B, Vol. 84, Issue 9 https://doi.org/10.1103/PhysRevB.84.094116	journal	September 2011
Phonon-phonon interactions in transition metals Chaput, Laurent; Togo, Atsushi; Tanaka, Isao Physical Review B, Vol. 84, Issue 9 https://doi.org/10.1103/PhysRevB.84.094302	journal	September 2011
Temperature and thickness evolution and epitaxial breakdown in highly strained BiFeO 3 thin films Damodaran, Anoop R.; Lee, Sungki; Karthik, J. Physical Review B, Vol. 85, Issue 2 https://doi.org/10.1103/PhysRevB.85.024113	journal	January 2012
Linear electro-optic effect in multiferroic BiFeO 3 thin films Sando, D.; Hermet, P.; Allibe, J. Physical Review B, Vol. 89, Issue 19 https://doi.org/10.1103/PhysRevB.89.195106	journal	May 2014
Tuning and optimizing properties of ferroelectric films grown on a single substrate: A first-principles-based study Gui, Zhigang; Bellaiche, L. Physical Review B, Vol. 91, Issue 2 https://doi.org/10.1103/PhysRevB.91.020102	journal	January 2015
Magnetic interactions in BiFeO 3 : A first-principles study Xu, Changsong; Xu, Bin; Dupé, Bertrand Physical Review B, Vol. 99, Issue 10 https://doi.org/10.1103/PhysRevB.99.104420	journal	March 2019
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
Strain-Induced Polarization Rotation in Epitaxial (001) BiFeO 3 Thin Films Jang, H. W.; Baek, S. H.; Ortiz, D. Physical Review Letters, Vol. 101, Issue 10 https://doi.org/10.1103/PhysRevLett.101.107602	journal	September 2008
Evidence for Room-Temperature Multiferroicity in a Compound with a Giant Axial Ratio Béa, H.; Dupé, B.; Fusil, S. Physical Review Letters, Vol. 102, Issue 21 https://doi.org/10.1103/PhysRevLett.102.217603	journal	May 2009
Electric-Field-Induced Paths in Multiferroic BiFeO 3 from Atomistic Simulations Lisenkov, S.; Rahmedov, D.; Bellaiche, L. Physical Review Letters, Vol. 103, Issue 4 https://doi.org/10.1103/PhysRevLett.103.047204	journal	July 2009
Large Piezoelectric Effect in Pb-Free Ceramics Liu, Wenfeng; Ren, Xiaobing Physical Review Letters, Vol. 103, Issue 25 https://doi.org/10.1103/PhysRevLett.103.257602	journal	December 2009
Ab Initio Indications for Giant Magnetoelectric Effects Driven by Structural Softness Wojdeł, Jacek C.; Íñiguez, Jorge Physical Review Letters, Vol. 105, Issue 3 https://doi.org/10.1103/PhysRevLett.105.037208	journal	July 2010
Engineering Polarization Rotation in a Ferroelectric Superlattice Sinsheimer, J.; Callori, S. J.; Bein, B. Physical Review Letters, Vol. 109, Issue 16 https://doi.org/10.1103/PhysRevLett.109.167601	journal	October 2012
Electric-Field Switching of Magnetic Topological Charge in Type-I Multiferroics Xu, Changsong; Chen, Peng; Tan, Hengxin Physical Review Letters, Vol. 125, Issue 3 https://doi.org/10.1103/PhysRevLett.125.037203	journal	July 2020
Finite-Temperature Properties of Pb ( Zr 1 − x Ti x ) O 3 Alloys from First Principles Bellaiche, L.; García, Alberto; Vanderbilt, David Physical Review Letters, Vol. 84, Issue 23 https://doi.org/10.1103/PhysRevLett.84.5427	journal	June 2000
Polarization Rotation via a Monoclinic Phase in the Piezoelectric 92% PbZn 1 / 3 Nb 2 / 3 O 3 -8% PbTiO 3 Noheda, B.; Cox, D. E.; Shirane, G. Physical Review Letters, Vol. 86, Issue 17 https://doi.org/10.1103/PhysRevLett.86.3891	journal	April 2001
First-Principles Determination of Electromechanical Responses of Solids under Finite Electric Fields Fu, Huaxiang; Bellaiche, L. Physical Review Letters, Vol. 91, Issue 5 https://doi.org/10.1103/PhysRevLett.91.057601	journal	July 2003
Conformal Miniaturization of Domains with Low Domain-Wall Energy: Monoclinic Ferroelectric States near the Morphotropic Phase Boundaries Jin, Y. M.; Wang, Y. U.; Khachaturyan, A. G. Physical Review Letters, Vol. 91, Issue 19 https://doi.org/10.1103/PhysRevLett.91.197601	journal	November 2003
Finite-Temperature Properties of Multiferroic BiFeO 3 Kornev, Igor A.; Lisenkov, S.; Haumont, R. Physical Review Letters, Vol. 99, Issue 22 https://doi.org/10.1103/PhysRevLett.99.227602	journal	November 2007
Contributions to the Piezoelectric Effect in Ferroelectric Single Crystals and Ceramics Damjanovic, Dragan Journal of the American Ceramic Society, Vol. 88, Issue 10 https://doi.org/10.1111/j.1551-2916.2005.00671.x	journal	October 2005
A Strain-Driven Morphotropic Phase Boundary in BiFeO₃ Zeches, R. J.; Rossell, M. D.; Zhang, J. X. Science, Vol. 326, Issue 5955, p. 977-980 https://doi.org/10.1126/science.1177046	journal	November 2009
Giant piezoelectricity of Sm-doped Pb(Mg _1/3 Nb _2/3 )O ₃ -PbTiO ₃ single crystals Li, Fei; Cabral, Matthew J.; Xu, Bin Science, Vol. 364, Issue 6437 https://doi.org/10.1126/science.aaw2781	journal	April 2019
Elastic anomalies in minerals due to structural phase transitions [Elastic anomalies in minerals due to structural phase transitions] Carpenter, Michael A.; Salje, Ekhard K. H. European Journal of Mineralogy, Vol. 10, Issue 4 https://doi.org/10.1127/ejm/10/4/0693	journal	July 1998
Strain Tuning of Ferroelectric Thin Films Schlom, Darrell G.; Chen, Long-Qing; Eom, Chang-Beom Annual Review of Materials Research, Vol. 37, Issue 1 https://doi.org/10.1146/annurev.matsci.37.061206.113016	journal	August 2007

Similar Records

Unraveling the origins of electromechanical response in mixed-phase Bismuth Ferrite

Journal Article · Mon Dec 31 23:00:00 EST 2012 · Physical Review B · OSTI ID:1088143

Origin of giant electric-field-induced strain in faulted alkali niobate films

Journal Article · Wed Jul 06 20:00:00 EDT 2022 · Nature Communications · OSTI ID:1877583

Strain-induced lead-free morphotropic phase boundary

Journal Article · Tue Aug 19 20:00:00 EDT 2025 · Nature Communications · OSTI ID:2587436

Related Subjects

36 MATERIALS SCIENCE
atomistic models
computational methods
ferroelectrics and multiferroics
surface interfaces and thin films

Anisotropic epitaxial stabilization of a low-symmetry ferroelectric with enhanced electromechanical response

Citation Formats

References (58)

Similar Records

Related Subjects