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Structural visualization of polarization fatigue in epitaxial ferroelectric oxide devices

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Abstract

Ferroelectric oxides, such as Pb(Zr,Ti)O3, are useful for electronic and photonic devices because of their ability to retain two stable polarization states, which can form the basis for memory and logic circuitry1. Requirements for long-term operation of practical devices such as non-volatile RAM (random access memory) include consistent polarization switching over many (more than 1012) cycles of the applied electric field, which represents a major challenge2. As switching is largely controlled by the motion and pinning of domain walls, it is necessary to develop suitable tools that can directly probe the ferroelectric domain structures in operating devices—thin-film structures with electrical contacts. A recently developed synchrotron X-ray microdiffraction technique complements existing microscopic probes, and allows us to visualize directly the evolution of polarization domains in ferroelectric devices, through metal or oxide electrodes, and with submicrometre spatial resolution. The images reveal two regimes of fatigue, depending on the magnitude of the electric field pulses driving the device: a low-field regime in which fatigue can be reversed with higher electric field pulses, and a regime at very high electric fields in which there is a non-reversible crystallographic relaxation of the epitaxial ferroelectric film.

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Figure 1: Polarization switching in a PZT thin-film capacitor.
Figure 2: Polarization fatigue.
Figure 3: Low-field fatigue.
Figure 4: High-field fatigue.

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References

  1. Scott, J.F. Ferroelectric Memories (Springer, Berlin, 2000).

    Book  Google Scholar 

  2. Tagantsev, A.K., Stolichnov, I., Colla, E.L. & Setter, N. Polarization fatigue in ferroelectric films: Basic experimental findings, phenomenological scenarios, and microscopic features. J. Appl. Phys. 90, 1387–1402 (2001).

    Article  CAS  Google Scholar 

  3. Dawber, M. & Scott, J.F. A model for fatigue in ferroelectric perovskite thin films. Appl. Phys. Lett. 76, 1060–1062 (2000).

    Article  CAS  Google Scholar 

  4. Larsen, P.K., Dormans, G.J.M., Taylor, D.J. & van Veldhoven, P.J. Ferroelectric properties and fatigue of PbZr0.51Ti0.49O3 thin films of varying thickness: Blocking layer model. J. Appl. Phys. 76, 2405–2413 (1994).

    Article  CAS  Google Scholar 

  5. Nagarajan, V. et al. Dynamics of ferroelastic domains in ferroelectric thin films. Nature Mater. 2, 43–47 (2002).

    Article  Google Scholar 

  6. Colla, E.L. et al. Direct observation of region by region suppression of the switchable polarization (fatigue) in Pb(Zr, Ti)O3 thin film capacitors with Pt electrodes. Appl. Phys. Lett. 72, 2763–2765 (1998).

    Article  CAS  Google Scholar 

  7. Gruverman, A., Auciello, O. & Tokumoto, H. Imaging and control of domain structures in ferroelectric thin films via scanning force microscopy. Annu. Rev. Mater. Sci. 28, 101–123 (1998).

    Article  CAS  Google Scholar 

  8. Rogan, R.C., Tamura, N., Swift, G.A. & Üstündag, E. Direct measurement of triaxial strain fields around ferroelectric domains using X-ray microdiffraction. Nature Mater. 2, 379–381 (2003).

    Article  CAS  Google Scholar 

  9. James, R.W. The Optical Principles of X-ray Diffraction 33 (Cornell Univ. Press, Ithaca, New York, 1965).

    Google Scholar 

  10. Wallace, C.A. The display of twinning in lithium niobate by x-ray diffraction topography. J. Appl. Crystallogr. 3, 546–547 (1970).

    Article  CAS  Google Scholar 

  11. Vreeland, T. & Speriousu, V.S. in Applications of X-ray Topographic Methods to Materials Science (eds Balibar, F. & Petroff, J.-F.) 501–509 (Plenum, New York, 1984).

    Google Scholar 

  12. Coster, D., Knol, K.S. & Prins, J.A. Difference in the intensities of x-ray reflection from the two sides of the 111 plane of zinc blende. Z. Phys. 63, 345–369 (1930).

    Article  CAS  Google Scholar 

  13. Colla, E.L., Tagantsev, A.K., Taylor D.V. & Kholkin, A.L. Fatigued state of the Pt-PZT-Pt system. Integr. Ferroelectr. 18, 19–28 (1997).

    Article  CAS  Google Scholar 

  14. Scott, J.F. & Pouligny, B.J. Raman spectroscopy of submicron KNO3 films. II. Fatigue and space-charge effects. J. Appl. Phys. 64, 1547–1561 (1988).

    Article  CAS  Google Scholar 

  15. Auciello, O. et al. Review of composition-structure-property relationships for PZT-based heterostructure capacitors. Integr. Ferroelectr. 6, 173–187 (1995).

    Article  CAS  Google Scholar 

  16. Eom, C.B. et al. Fabrication and properties of epitaxial ferroelectric heterostructures with (SrRuO3) isotropic metallic oxide electrodes. Appl. Phys. Lett. 63, 2570–2572 (1993).

    Article  CAS  Google Scholar 

  17. Duiker, H.M. et al. Fatigue and switching in ferroelectric memories: theory and experiment. J. Appl. Phys. 68, 5783–5791 (1990).

    Article  CAS  Google Scholar 

  18. Thompson, C. et al. X-ray scattering evidence for the structural nature of fatigue in epitaxial Pb(Zr, Ti)O3 films. Appl. Phys. Lett. 78, 3511–3513 (2001).

    Article  CAS  Google Scholar 

  19. Jiang, A. et al. Studies of switching kinetics in ferroelectric thin films. Jpn. J. Appl. Phys. 42, 6973–6982 (2003).

    Article  CAS  Google Scholar 

  20. Eom, C.B. et al. Single-crystal epitaxial thin films of the isotropic metallic oxides Sr1−xCaxRuO3 (0 ≤ x ≤ 1). Science 258, 1766–1769 (1992).

    Article  CAS  Google Scholar 

  21. Noheda, B. et al. A monoclinic ferroelectric phase in the Pb(Zr1−xTix)O3 solid solution. Appl. Phys. Lett. 74, 2059–2061 (1999).

    Article  CAS  Google Scholar 

  22. Grossmann, M. et al. Correlation between switching and fatigue in PbZr0.3Ti0.7O3 thin films. Appl. Phys. Lett. 77, 1894–1896 (2000).

    Article  CAS  Google Scholar 

  23. Cai, Z., Lai, B., Xiao, Y. & Xu, S. An X-ray diffraction microscope at the Advanced Photon Source. J. Phys. IV 104, 17–20 (2003).

    CAS  Google Scholar 

  24. Lai, B. et al. Hard X-ray phase zone plate fabricated by lithographic techniques. Appl. Phys. Lett. 61, 1877–1879 (1992).

    Article  CAS  Google Scholar 

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Acknowledgements

This work was supported by the National Science Foundation through the University of Wisconsin Materials Research Science and Engineering Center (grant number DMR-0079983) and grant no. DMR-0313764 (C.B.E.). Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences (contract number W-31-109-Eng-38). E.D. acknowledges support from the US Department of Energy (grant numbers DE-FG02-03ER46023 and DE-FG02-00ER15031), and from the NSF FOCUS physics frontier centre.

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Correspondence to Paul G. Evans.

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Do, DH., Evans, P., Isaacs, E. et al. Structural visualization of polarization fatigue in epitaxial ferroelectric oxide devices. Nature Mater 3, 365–369 (2004). https://doi.org/10.1038/nmat1122

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