Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Resonant domain-wall-enhanced tunable microwave ferroelectrics

Abstract

Ordering of ferroelectric polarization1 and its trajectory in response to an electric field2 are essential for the operation of non-volatile memories3, transducers4 and electro-optic devices5. However, for voltage control of capacitance and frequency agility in telecommunication devices, domain walls have long been thought to be a hindrance because they lead to high dielectric loss and hysteresis in the device response to an applied electric field6. To avoid these effects, tunable dielectrics are often operated under piezoelectric resonance conditions, relying on operation well above the ferroelectric Curie temperature7, where tunability is compromised. Therefore, there is an unavoidable trade-off between the requirements of high tunability and low loss in tunable dielectric devices, which leads to severe limitations on their figure of merit. Here we show that domain structure can in fact be exploited to obtain ultralow loss and exceptional frequency selectivity without piezoelectric resonance. We use intrinsically tunable materials with properties that are defined not only by their chemical composition, but also by the proximity and accessibility of thermodynamically predicted strain-induced, ferroelectric domain-wall variants8. The resulting gigahertz microwave tunability and dielectric loss are better than those of the best film devices by one to two orders of magnitude and comparable to those of bulk single crystals. The measured quality factors exceed the theoretically predicted zero-field intrinsic limit owing to domain-wall fluctuations, rather than field-induced piezoelectric oscillations, which are usually associated with resonance. Resonant frequency tuning across the entire L, S and C microwave bands (1–8 gigahertz) is achieved in an individual device—a range about 100 times larger than that of the best intrinsically tunable material. These results point to a rich phase space of possible nanometre-scale domain structures that can be used to surmount current limitations, and demonstrate a promising strategy for obtaining ultrahigh frequency agility and low-loss microwave devices.

Access options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

Fig. 1: Design of a MDVM and its microwave dielectric tunability.
Fig. 2: Microwave spectroscopy results revealing field-dependent resonant domain-wall spectral signatures of ultralow loss and tunable resonant performance.
Fig. 3: Molecular dynamics simulation of Q.

References

  1. 1.

    Merz, W. J. Domain formation and domain wall motions in ferroelectric BaTiO3 single crystals. Phys. Rev. 95, 690–698 (1954).

    ADS  Article  CAS  Google Scholar 

  2. 2.

    Xu, R., Liu, S., Grinberg, I., Karthik, J., Damodaran, A. R., Rappe, A. M. & Martin, L. W. Ferroelectric polarization reversal via successive ferroelastic transitions. Nat. Mater. 14, 79–86 (2015).

    ADS  Article  PubMed  CAS  Google Scholar 

  3. 3.

    Chanthbouala, A. et al. Solid-state memories based on ferroelectric tunnel junctions. Nat. Nanotechnol. 7, 101–104 (2012).

    ADS  Article  CAS  Google Scholar 

  4. 4.

    Muralt, P. Ferroelectric thin films for micro-sensors and actuators: a review. J. Micromech. Microeng. 10, 136–146 (2000).

    ADS  Article  CAS  Google Scholar 

  5. 5.

    Wessels, B. W. Ferroelectric epitaxial thin films for integrated optics. Annu. Rev. Mater. Res. 37, 659–679 (2007).

    ADS  Article  CAS  Google Scholar 

  6. 6.

    Arlt, G., Böttger, U. & Witte, S. Dielectric dispersion of ferroelectric ceramics and single crystals at microwave frequencies. Ann. Phys. 506, 578–588 (1994).

    Article  Google Scholar 

  7. 7.

    York, B. in Multifunctional Adaptive Microwave Circuits and Systems (eds Steer, M. & Palmer, W. D.) Ch. 6 (SciTech Publishing, Raleigh, 2006).

  8. 8.

    Pertsev, N. A., Zembilgotov, A. G. & Tagantsev, A. K. Effect of mechanical boundary conditions on phase diagrams of epitaxial ferroelectric thin films. Phys. Rev. Lett. 80, 1988–1991 (1998).

    ADS  Article  CAS  Google Scholar 

  9. 9.

    Lee, C.-H. et al. Exploiting dimensionality and defect mitigation to create tunable microwave dielectrics. Nature 502, 532–536 (2013).

    ADS  Article  PubMed  CAS  Google Scholar 

  10. 10.

    Damodaran, A. R., Breckenfeld, E., Chen, Z., Lee, S. & Martin, L. W. Enhancement of ferroelectric Curie temperature in BaTiO3 films via strain-induced defect dipole alignment. Adv. Mater. 26, 6341–6347 (2014).

    Article  PubMed  CAS  Google Scholar 

  11. 11.

    Damodaran, A. R. et al. Nanoscale structure and mechanism for enhanced electromechanical response of highly strained BiFeO3 thin films. Adv. Mater. 23, 3170–3175 (2011).

    Article  PubMed  CAS  Google Scholar 

  12. 12.

    Prosandeev, S., Yang, Y., Paillard, C. & Bellaiche, L. Displacement current in domain walls of bismuth ferrite. npj Comput. Mater. 4, 8 (2018).

    Google Scholar 

  13. 13.

    Wang, Y. L., Tagantsev, A. K., Damjanovic, D. & Setter, N. Giant domain wall contribution to the dielectric susceptibility in BaTiO3. Appl. Phys. Lett. 91, 062905 (2007).

    ADS  Article  CAS  Google Scholar 

  14. 14.

    Tagantsev, A. K., Sherman, V. O., Astafiev, K. F., Venkatesh, J. & Setter, N. Ferroelectric materials for microwave tunable applications. J. Electroceram. 11, 5–66 (2003).

    Article  CAS  Google Scholar 

  15. 15.

    Matzen, S. et al. Super switching and control of in-plane ferroelectric nanodomains in strained thin films. Nat. Commun. 5, 4415 (2014).

    Article  PubMed  CAS  Google Scholar 

  16. 16.

    Griggio, F. et al. Composition dependence of local piezoelectric nonlinearity in (0.3)Pb(Ni0.33Nb0.67)O3-(0.7)Pb(ZrxTi1−x)O3 films. J. Appl. Phys. 110, 044109 (2011).

    ADS  Article  CAS  Google Scholar 

  17. 17.

    Meyers, C. J. G., Freeze, C. R., Stemmer, S. & York, R. A. (Ba, Sr)TiO3 tunable capacitors with RF commutation quality factors exceeding 6000. Appl. Phys. Lett. 109, 112902 (2016).

    ADS  Article  CAS  Google Scholar 

  18. 18.

    Vorobiev, A., Gevorgian, S., Löffler, M. & Olsson, E. Correlations between microstructure and Q-factor of tunable thin film bulk acoustic wave resonators. J. Appl. Phys. 110, 054102 (2011).

    ADS  Article  CAS  Google Scholar 

  19. 19.

    Budimir, M., Damjanovic, D. & Setter, N. Extension of the dielectric tunability range in ferroelectric materials by electric bias field antiparallel to polarization. Appl. Phys. Lett. 88, 082903 (2006).

    ADS  Article  CAS  Google Scholar 

  20. 20.

    Rojac, T., Bencan, A., Drazic, G., Kosec, M. & Damjanovic, D. Piezoelectric nonlinearity and frequency dispersion of the direct piezoelectric response of BiFeO3 ceramics. J. Appl. Phys. 112, 064114 (2012).

    ADS  Article  CAS  Google Scholar 

  21. 21.

    Zuo, C., Der Spiegel, J. V. & Piazza, G. 1.05-GHz cmos oscillator based on lateral- field-excited piezoelectric AlN contour-mode MEMS resonators. IEEE Trans. Ultrason. Ferroelectr. Freq. Control 57, 82–87 (2010).

    Article  PubMed  Google Scholar 

  22. 22.

    Gong, S., Kuo, N. K. & Piazza, G. GHz high-Q lateral overmoded bulk acoustic-wave resonators using epitaxial SiC thin film. J. Microelectromech. Syst. 21, 253–255 (2012).

    Article  CAS  Google Scholar 

  23. 23.

    Rinaldi, M., Zuniga, C., Zuo, C. & Piazza, G. Super-high-frequency two-port AlN contour-mode resonators for RF applications. IEEE Trans. Ultrason. Ferroelectr. Freq. Control 57, 38–45 (2010).

    Article  PubMed  Google Scholar 

  24. 24.

    Rinaldi, M., Zuniga, C. & Piazza, G. 5–10 GHz AlN contour-mode nanoelectromechanical resonators. In 2009 IEEE 22nd International Conference on Micro Electro Mechanical Systems 916–919 (IEEE, 2009).

  25. 25.

    Krupka, J., Tobar, M. E., Hartnett, J. G., Cros, D. & Le Floch, J. M. Extremely high-Q factor dielectric resonators for millimeter-wave applications. IEEE Trans. Microw. Theory Tech. 53, 702–712 (2005).

    ADS  Article  Google Scholar 

  26. 26.

    Hartnett, J. G., Tobar, M. E., Ivanov, E. N. & Krupka, J. Room temperature measurement of the anisotropic loss tangent of sapphire using the whispering gallery mode technique. IEEE Trans. Ultrason. Ferroelectr. Freq. Control 53, 34–38 (2006).

    Article  PubMed  Google Scholar 

  27. 27.

    Magnusson, E. B. et al. Surface acoustic wave devices on bulk ZnO crystals at low temperature. Appl. Phys. Lett. 106, 063509 (2015).

    ADS  Article  CAS  Google Scholar 

  28. 28.

    Vendik, I. B., Vendik, O. G. & Kollberg, E. L. Commutation quality factor of two-state switchable devices. IEEE Trans. Microw. Theory Tech. 48, 802–808 (2000).

    ADS  Article  Google Scholar 

  29. 29.

    Berge, J. & Gevorgian, S. Tunable bulk acoustic wave resonators based on Ba0.25Sr0.75TiO3 thin films and a HfO2/SiO2 Bragg reflector. IEEE Trans. Ultrason. Ferroelectr. Freq. Control 58, 2768–2771 (2011).

    Article  PubMed  Google Scholar 

  30. 30.

    Gevorgian, S. S., Tagantsev, A. K. & Vorobiev, A. K. Tunable Film Bulk Acoustic Wave Resonators (Springer, New York, 2013).

    Book  Google Scholar 

  31. 31.

    Hoshina, T. et al. Domain size effect on dielectric properties of barium titanate ceramics. Jpn. J. Appl. Phys. 47, 7607–7611 (2008).

    ADS  Article  CAS  Google Scholar 

  32. 32.

    Gammaitoni, L., Hänggi, P., Jung, P. & Marchesoni, F. Stochastic resonance. Rev. Mod. Phys. 70, 223–287 (1998).

    ADS  Article  CAS  Google Scholar 

  33. 33.

    Akhiezer, A. On the absorption of sound in solids. J. Phys. USSR 1, 277 (1939).

    MATH  Google Scholar 

  34. 34.

    Shirokov, V. B., Yuzkuk, Yu. I., Dkhil, B. & Lemanov, V. V. Phenomenological theory of phase transitions in epitaxial BaxSr1−xTiO3 thin films. Phys. Rev. B 79, 144118 (2009).

    ADS  Article  CAS  Google Scholar 

  35. 35.

    Qi, Y., Liu, S., Grinberg, I. & Rappe, A. M. Atomistic description for temperature-driven phase transitions in BaTiO3. Phys. Rev. B 94, 134308 (2016).

    ADS  Article  CAS  Google Scholar 

Download references

Acknowledgements

Work at Drexel University and the University of California at Berkeley was supported in part by the US National Science Foundation (NSF) and the Semiconductor Research Corporation under the ‘Nanoelectronics in 2020 and Beyond’ programme grant number DMR 1124696 and by the Materials Science Division of the US Army Research Office (ARO). Z.G. and G.X. acknowledge support from the ARO under grant number W911NF-14-1-0500. A.P. and A.A.P. acknowledge support from the NSF under grant number IIP 1549668. A.W.-C. acknowledges support from the NSF under grant number DMR 1608887. C.J.H. acknowledges support from the Office of Naval Research under grant number N00014-15-11-2170. J.E.S. acknowledges support from the Air Force Office of Scientific Research under grant number FA9550-13-1-012. I.G., A.S., H.B., J.E.S. and G.X. acknowledge support from the NSF–BSF (US–Israel Binational Science Foundation) joint programme under grant numbers BSF 2016637 and CBET 1705440. S.P. and A.R.D. acknowledge support from the ARO under grant number W911NF-14-1-0104. A.R.D. also acknowledges the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under award number DE-SC-0012375 for the development of the BST materials. A.D. acknowledges support from the NSF under grant number DMR 1708615. S.S. acknowledges support from the NSF under grant number DMR 1608938. L.W.M. acknowledges support from the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC02-05-CH11231: Materials Project programme KC23MP for the development of new functional materials. R.A.Y. and C.J.G.M. acknowledge support from ARO under grant number W911NF-14-1-0335. Numerical GLD and phase-field simulations were carried out on Proteus, a computer cluster supported by the Drexel University Research Computing Facility.

Reviewer information

Nature thanks S. Prosandeev, A. Vorobiev and the other anonymous reviewer(s) for their contribution to the peer review of this work.

Author information

Affiliations

Authors

Contributions

Z.G. and J.E.S. conceived the idea and, together with I.G., proposed the mechanism for high Q. Z.G. and J.E.S. developed and implemented the GLD model; G.X., Z.G. and J.E.S. implemented the phase-field model; and A.S., S.L. and I.G. carried out the molecular dynamics simulations and analysis of the molecular dynamics data. H.B. and I.G. developed the stochastic oscillator model. S.P., A.R.D., A.D., Z.G., L.W.M. and J.E.S. designed the growth experiments, and Z.G., I.G. and J.E.S. formulated the interpretation of the experimental data. A.D., A.R.D., S.P. and Z.G. carried out the film synthesis and its optimization. L.W. and P.K.D. produced the solid-state sources. S.P., A.D. and Z.G. carried out X-ray diffraction measurements, X-ray reflectivity analysis and reciprocal space mapping. Z.G., A.D. and S.P. carried out piezoresponse force microscopy analysis. C.J.G.M. designed the microwave devices, carried out film processing and device fabrication and performed microwave measurements and analysis, which were supervised by R.A.Y. Assistance in microwave device design, fabrication, measurements and analysis was provided by A.P., A.A.P. and A.W.-C. The theoretical, experimental and computational modeling aspects of the project were overseen together by I.G., R.A.Y., L.W.M. and J.E.S. All authors contributed to the data analysis. Z.G., I.G. and J.E.S. wrote the manuscript. Z.G., G.X., S.P., A.S., A.D., A.R.D., S.S., C.J.G.M., R.A.Y., I.G., L.W.M. and J.E.S. edited and commented on the manuscript.

Corresponding author

Correspondence to Jonathan E. Spanier.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Ginzburg–Landau–Devonshire-based derivation of free energies and field-tuned dielectric susceptibility in domain wall variant phases, description of phase field model, table and illustrations of domain wall variants, X-ray diffraction and reciprocal space mapping data, additional microwave-band n, Q, and S parameter data; additional molecular dynamics calculation results and stochastic model calculations results.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Gu, Z., Pandya, S., Samanta, A. et al. Resonant domain-wall-enhanced tunable microwave ferroelectrics. Nature 560, 622–627 (2018). https://doi.org/10.1038/s41586-018-0434-2

Download citation

Further reading

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing