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Title: Non-conventional mechanism of ferroelectric fatigue via cation migration

Abstract

The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling. Multiple microscopic models explaining fatigue have been suggested; however, the chemical origins remain poorly understood. Here, we utilize multimodal chemical imaging that combines atomic force microscopy with time-of-flight secondary mass spectrometry to explore the chemical phenomena associated with fatigue in PbZr0.2Ti0.8O3 (PZT) thin films. Investigations reveal that the degradation of ferroelectric properties is correlated with a local chemical change and migration of electrode ions into the PZT structure. Density functional theory simulations support the experimental results and demonstrate stable doping of the thin surface PZT layer with copper ions, leading to a decrease in the spontaneous polarization. Overall, the performed research allows for the observation and understanding of the chemical phenomena associated with polarization cycling and their effects on ferroelectric functionality.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Sungkyunkwan Univ., Suwon (Republic of Korea)
  3. Xidian Univ., Xi’an (China)
  4. Univ. of Warwick, Coventry (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1542232
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ievlev, Anton V., KC, Santosh, Vasudevan, Rama K., Kim, Yunseok, Lu, Xiaoli, Alexe, Marin, Cooper, Valentino R., Kalinin, Sergei V., and Ovchinnikova, Olga S. Non-conventional mechanism of ferroelectric fatigue via cation migration. United States: N. p., 2019. Web. https://doi.org/10.1038/s41467-019-11089-w.
Ievlev, Anton V., KC, Santosh, Vasudevan, Rama K., Kim, Yunseok, Lu, Xiaoli, Alexe, Marin, Cooper, Valentino R., Kalinin, Sergei V., & Ovchinnikova, Olga S. Non-conventional mechanism of ferroelectric fatigue via cation migration. United States. https://doi.org/10.1038/s41467-019-11089-w
Ievlev, Anton V., KC, Santosh, Vasudevan, Rama K., Kim, Yunseok, Lu, Xiaoli, Alexe, Marin, Cooper, Valentino R., Kalinin, Sergei V., and Ovchinnikova, Olga S. Thu . "Non-conventional mechanism of ferroelectric fatigue via cation migration". United States. https://doi.org/10.1038/s41467-019-11089-w. https://www.osti.gov/servlets/purl/1542232.
@article{osti_1542232,
title = {Non-conventional mechanism of ferroelectric fatigue via cation migration},
author = {Ievlev, Anton V. and KC, Santosh and Vasudevan, Rama K. and Kim, Yunseok and Lu, Xiaoli and Alexe, Marin and Cooper, Valentino R. and Kalinin, Sergei V. and Ovchinnikova, Olga S.},
abstractNote = {The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling. Multiple microscopic models explaining fatigue have been suggested; however, the chemical origins remain poorly understood. Here, we utilize multimodal chemical imaging that combines atomic force microscopy with time-of-flight secondary mass spectrometry to explore the chemical phenomena associated with fatigue in PbZr0.2Ti0.8O3 (PZT) thin films. Investigations reveal that the degradation of ferroelectric properties is correlated with a local chemical change and migration of electrode ions into the PZT structure. Density functional theory simulations support the experimental results and demonstrate stable doping of the thin surface PZT layer with copper ions, leading to a decrease in the spontaneous polarization. Overall, the performed research allows for the observation and understanding of the chemical phenomena associated with polarization cycling and their effects on ferroelectric functionality.},
doi = {10.1038/s41467-019-11089-w},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {7}
}

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Cited by: 3 works
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Figures / Tables:

Fig. 1 Fig. 1: AFM studies of PZT nanocapacitors. a Topography of the pristine sample. b–g Polarization switching of a single capacitor via an AFM tip: b, e before switching; c, f switching with +4 V; d, g back switching with −4 V. Signals of b–d topography and e–g PFM phases

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Works referenced in this record:

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Data encoding based on the shape of the ferroelectric domains produced by using a scanning probe microscope tip
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    Works referencing / citing this record:

    Nanoscale Observation of Time-Dependent Domain Wall Pinning as the Origin of Polarization Fatigue
    journal, March 2012

    • Yang, Sang Mo; Kim, Tae Heon; Yoon, Jong-Gul
    • Advanced Functional Materials, Vol. 22, Issue 11
    • DOI: 10.1002/adfm.201102685

    Universality of Polarization Switching Dynamics in Ferroelectric Capacitors Revealed by 5D Piezoresponse Force Microscopy
    journal, April 2013

    • Kim, Yunseok; Lu, Xiaoli; Jesse, Stephen
    • Advanced Functional Materials, Vol. 23, Issue 32
    • DOI: 10.1002/adfm.201300079

    Structural Changes Underlying Field-Cycling Phenomena in Ferroelectric HfO 2 Thin Films
    journal, July 2016

    • Grimley, Everett D.; Schenk, Tony; Sang, Xiahan
    • Advanced Electronic Materials, Vol. 2, Issue 9
    • DOI: 10.1002/aelm.201600173

    Imaging mass spectrometry
    journal, January 2007

    • McDonnell, Liam A.; Heeren, Ron M. A.
    • Mass Spectrometry Reviews, Vol. 26, Issue 4
    • DOI: 10.1002/mas.20124

    Ferroelectric materials for electromechanical transducer applications
    journal, February 1996


    Patterned nano-domains in PMN-PT single crystals
    journal, January 2018


    Microstructural modifications of ferroelectric lead zirconate titanate ceramics due to bipolar electric fatigue
    journal, December 2002

    • Nuffer, Jürgen; Lupascu, Doru C.; Glazounov, Alexandre
    • Journal of the European Ceramic Society, Vol. 22, Issue 13
    • DOI: 10.1016/s0955-2219(02)00017-1

    Chemical State Evolution in Ferroelectric Films during Tip-Induced Polarization and Electroresistive Switching
    journal, October 2016

    • Ievlev, Anton V.; Maksymovych, Petro; Trassin, Morgan
    • ACS Applied Materials & Interfaces, Vol. 8, Issue 43
    • DOI: 10.1021/acsami.6b10784

    Nanoscale Electrochemical Phenomena of Polarization Switching in Ferroelectrics
    journal, October 2018

    • Ievlev, Anton V.; Brown, Chance C.; Agar, Joshua C.
    • ACS Applied Materials & Interfaces, Vol. 10, Issue 44
    • DOI: 10.1021/acsami.8b13034

    Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides
    journal, June 2018

    • Sharma, Yogesh; Balachandran, Janakiraman; Sohn, Changhee
    • ACS Nano, Vol. 12, Issue 7
    • DOI: 10.1021/acsnano.8b03031

    Imaging with Mass Spectrometry
    journal, October 1999

    • Pacholski, M. L.; Winograd, N.
    • Chemical Reviews, Vol. 99, Issue 10
    • DOI: 10.1021/cr980137w

    Lead zirconate titanate thin films directly on copper electrodes for ferroelectric, dielectric and piezoelectric applications
    journal, February 2005

    • Kingon, Angus I.; Srinivasan, Sudarsan
    • Nature Materials, Vol. 4, Issue 3, p. 233-237
    • DOI: 10.1038/nmat1334

    Individually addressable epitaxial ferroelectric nanocapacitor arrays with near Tb inch−2 density
    journal, June 2008


    Intermittency, quasiperiodicity and chaos in probe-induced ferroelectric domain switching
    journal, November 2013

    • Ievlev, A. V.; Jesse, S.; Morozovska, A. N.
    • Nature Physics, Vol. 10, Issue 1, p. 59-66
    • DOI: 10.1038/nphys2796

    Data encoding based on the shape of the ferroelectric domains produced by using a scanning probe microscope tip
    journal, January 2015

    • Ievlev, Anton V.; Kalinin, Sergei V.
    • Nanoscale, Vol. 7, Issue 25
    • DOI: 10.1039/c5nr02443a

    Nanoscale investigation of fatigue effects in Pb(Zr,Ti)O 3 films
    journal, November 1996

    • Gruverman, A.; Auciello, O.; Tokumoto, H.
    • Applied Physics Letters, Vol. 69, Issue 21
    • DOI: 10.1063/1.117957

    Injection-controlled size effect on switching of ferroelectric thin films
    journal, March 1999

    • Tagantsev, A. K.; Stolichnov, I. A.
    • Applied Physics Letters, Vol. 74, Issue 9
    • DOI: 10.1063/1.123539

    A model for fatigue in ferroelectric perovskite thin films
    journal, February 2000

    • Dawber, Matthew; Scott, J. F.
    • Applied Physics Letters, Vol. 76, Issue 8
    • DOI: 10.1063/1.125938

    Downscaling of Pb(Zr,Ti)O3 film thickness for low-voltage ferroelectric capacitors: Effect of charge relaxation at the interfaces
    journal, August 2000

    • Stolichnov, I.; Tagantsev, A.; Colla, E.
    • Journal of Applied Physics, Vol. 88, Issue 4
    • DOI: 10.1063/1.1305854

    Polarization fatigue in ferroelectric films: Basic experimental findings, phenomenological scenarios, and microscopic features
    journal, August 2001

    • Tagantsev, A. K.; Stolichnov, I.; Colla, E. L.
    • Journal of Applied Physics, Vol. 90, Issue 3
    • DOI: 10.1063/1.1381542

    Tbit/inch2 ferroelectric data storage based on scanning nonlinear dielectric microscopy
    journal, December 2002

    • Cho, Yasuo; Fujimoto, Kenjiro; Hiranaga, Yoshiomi
    • Applied Physics Letters, Vol. 81, Issue 23
    • DOI: 10.1063/1.1526916

    Switching spectroscopy piezoresponse force microscopy of ferroelectric materials
    journal, February 2006

    • Jesse, Stephen; Baddorf, Arthur P.; Kalinin, Sergei V.
    • Applied Physics Letters, Vol. 88, Issue 6
    • DOI: 10.1063/1.2172216

    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
    • DOI: 10.1063/1.2336999

    Device modeling of ferroelectric capacitors
    journal, December 1990

    • Miller, S. L.; Nasby, R. D.; Schwank, J. R.
    • Journal of Applied Physics, Vol. 68, Issue 12
    • DOI: 10.1063/1.346845

    Fatigue and switching in ferroelectric memories: Theory and experiment
    journal, December 1990

    • Duiker, H. M.; Beale, P. D.; Scott, J. F.
    • Journal of Applied Physics, Vol. 68, Issue 11
    • DOI: 10.1063/1.346948

    Quantitative measurement of space‐charge effects in lead zirconate‐titanate memories
    journal, July 1991

    • Scott, J. F.; Araujo, C. A.; Melnick, B. M.
    • Journal of Applied Physics, Vol. 70, Issue 1
    • DOI: 10.1063/1.350286

    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
    • DOI: 10.1063/1.357589

    Polarization suppression in Pb(Zr,Ti)O 3 thin films
    journal, June 1995

    • Warren, W. L.; Dimos, D.; Tuttle, B. A.
    • Journal of Applied Physics, Vol. 77, Issue 12
    • DOI: 10.1063/1.359083

    Fatigue of Pb(Zr0.53Ti0.47)O3 ferroelectric thin films
    journal, June 1998

    • Du, Xiaofeng; Chen, I. -Wei
    • Journal of Applied Physics, Vol. 83, Issue 12
    • DOI: 10.1063/1.367953

    Wake-up effects in Si-doped hafnium oxide ferroelectric thin films
    journal, November 2013

    • Zhou, Dayu; Xu, Jin; Li, Qing
    • Applied Physics Letters, Vol. 103, Issue 19
    • DOI: 10.1063/1.4829064

    Domain disruption and defect accumulation during unipolar electric fatigue in a BZT-BCT ceramic
    journal, December 2017

    • Fan, Zhongming; Zhou, Chao; Ren, Xiaobing
    • Applied Physics Letters, Vol. 111, Issue 25
    • DOI: 10.1063/1.5008619

    Recent achievements in domain engineering in lithium niobate and lithium tantalate
    journal, January 2001


    Model of ferroelectric fatigue due to defect/domain interactions
    journal, December 1993


    Fatigued state of the Pt-PZT-Pt system
    journal, September 1997


    A critical study of defect migration and ferroelectric fatigue in lead zirconate titanate thin film capacitors under extreme temperatures
    journal, September 1997


    Piezoresponse force microscopy (PFM)
    journal, November 2011


    Nanoscale ferroelectrics: processing, characterization and future trends
    journal, July 2006


    Local polarization dynamics in ferroelectric materials
    journal, April 2010

    • Kalinin, Sergei V.; Morozovska, Anna N.; Chen, Long Qing
    • Reports on Progress in Physics, Vol. 73, Issue 5, Article No. 056502
    • DOI: 10.1088/0034-4885/73/5/056502

    Subtractive fabrication of ferroelectric thin films with precisely controlled thickness
    journal, February 2018

    • Ievlev, Anton V.; Chyasnavichyus, Marius; Leonard, Donovan N.
    • Nanotechnology, Vol. 29, Issue 15
    • DOI: 10.1088/1361-6528/aaac9b

    Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
    journal, October 1996


    Special quasirandom structures to study the ( K 0.5 Na 0.5 ) Nb O 3 random alloy
    journal, July 2014


    Special quasirandom structures
    journal, July 1990


    Comparative Study of Hydrogen- and Deuterium-Induced Degradation of Ferroelectric (Pb,La)(Zr,Ti)O 3 Capacitors Using Time-of-Flight Secondary Ion Measurement
    journal, October 2016

    • Takada, Yoko; Okamoto, Naoki; Saito, Takeyasu
    • IEEE Transactions on Ultrasonics, Ferroelectrics, and Frequency Control, Vol. 63, Issue 10
    • DOI: 10.1109/tuffc.2016.2593585

    Applications of Modern Ferroelectrics
    journal, February 2007


    Polarization Fatigue Characteristics of Sol-Gel Ferroelectric P b ( Z r 0.4 T i 0.6 ) O 3 Thin-Film Capacitors
    journal, July 1994

    • Mihara, Takashi; Watanabe, Hitoshi; Araujo, Carlos A. Paz de
    • Japanese Journal of Applied Physics, Vol. 33, Issue Part 1, No. 7A
    • DOI: 10.1143/jjap.33.3996

    The Effects of La and Nb Modification on Fatigue and Retention Properties of Pb(Ti, Zr)O3 Thin-Film Capacitors
    journal, September 1997

    • Aoki, Katsuhiro; Fukuda, Yukio
    • Japanese Journal of Applied Physics, Vol. 36, Issue Part 2, No. 9A/B
    • DOI: 10.1143/jjap.36.l1195

    Increase in Switching Charge of Ferroelectric SrBi 2 Ta 2 O 9 Thin Films with Polarization Reversal
    journal, September 2000

    • Okamura, Soichiro; Takaoka, Masaki; Nishida, Takashi
    • Japanese Journal of Applied Physics, Vol. 39, Issue Part 1, No. 9B
    • DOI: 10.1143/jjap.39.5481

    Quasi-phase-matched optical parametric oscillation with periodically poled stoichiometric LiTaO_3
    journal, January 2000

    • Hatanaka, Takaaki; Nakamura, Koichiro; Taniuchi, Tetsuo
    • Optics Letters, Vol. 25, Issue 9
    • DOI: 10.1364/ol.25.000651

    Integrated Optical Devices in Lithium Niobate
    journal, January 2008

    • Sohler, Wolfgang; Hu, Hui; Ricken, Raimund
    • Optics and Photonics News, Vol. 19, Issue 1
    • DOI: 10.1364/opn.19.1.000024

    Fatigue of ferroelectric PbZr x Ti y O 3 capacitors with Ru and RuO x electrodes
    journal, January 1993

    • Bernstein, S. D.; Wong, T. Y.; Kisler, Yanina
    • Journal of Materials Research, Vol. 8, Issue 1
    • DOI: 10.1557/jmr.1993.0012

    Self‐Assembled Room Temperature Multiferroic BiFeO 3 ‐LiFe 5 O 8 Nanocomposites
    journal, October 2019

    • Sharma, Yogesh; Agarwal, Radhe; Collins, Liam
    • Advanced Functional Materials, Vol. 30, Issue 3
    • DOI: 10.1002/adfm.201906849

    Investigation of AFM-based machining of ferroelectric thin films at the nanoscale
    journal, January 2020

    • Zhang, Fengyuan; Edwards, David; Deng, Xiong
    • Journal of Applied Physics, Vol. 127, Issue 3
    • DOI: 10.1063/1.5133018

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.