Abstract
Strong light–matter interaction constitutes the bedrock of all photonic applications, empowering material elements with the ability to create and mediate interactions of light with light. Amidst the quest to identify new agents facilitating such efficient light–matter interactions, a class of promising materials has emerged, featuring highly unusual properties deriving from their dielectric constant ε being equal, or at least very close, to zero. Works so far have shown that the enhanced nonlinear optical effects displayed in this epsilon-near-zero (ENZ) regime make it possible to create ultrafast albeit transient optical switches. An outstanding question, however, relates to whether one could use the amplification of light–matter interactions at the ENZ conditions to achieve permanent switching. Here we demonstrate that an ultrafast excitation under ENZ conditions can induce permanent all-optical reversal of ferroelectric polarization between different stable states. Our reliance on ENZ conditions that naturally emerge from the solid’s ionic lattice suggests that the demonstrated mechanism of reversal is truly universal, being capable of permanently switching order parameters in a wide variety of systems.
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Data availability
The data supporting the findings of this study are available within the article and its Supplementary Information. Additional data can be obtained from the authors upon a reasonable request. Source Data are provided with this paper.
References
Scott, J. F. Applications of modern ferroelectrics. Science 315, 954–959 (2007).
Sharma, P. et al. Nonvolatile ferroelectric domain wall memory. Sci. Adv. 3, e1700512 (2017).
Jiang, J. et al. Temporary formation of highly conducting domain walls for non-destructive read-out of ferroelectric domain-wall resistance switching memories. Nat. Mater. 17, 49–56 (2018).
Petritz, A. et al. Imperceptible energy harvesting device and biomedical sensor based on ultraflexible ferroelectric transducers and organic diodes. Nat. Commun. 12, 2399 (2021).
Chanthbouala, A. et al. A ferroelectric memristor. Nat. Mater. 11, 860–864 (2012).
Wei, X. et al. Progress on emerging ferroelectric materials for energy harvesting, storage and conversion. Adv. Energy Mater. 12, 2201199 (2022).
Tagantsev, A.K., Cross, L.E. & Fousek, J. Domains in Ferroic Crystals and Thin Films (Springer, 2010).
Fiebig, M., Lottermoser, T., Meier, D. & Trassin, M. The evolution of multiferroics. Nat. Rev. Mater. 1, 16046 (2016).
von Hippel, A. Ferroelectricity, domain structure, and phase transitions of barium titanate. Rev. Mod. Phys. 22, 221–237 (1950).
Harada, J., Pedersen, T. & Barnea, Z. X-ray and neutron diffraction study of tetragonal barium titanate. Acta Cryst. A 26, 336–344 (1970).
Merz, W. J. Domain formation and domain wall motions in ferroelectric BaTiO3 single crystals. Phys. Rev. 95, 690–698 (1954).
Servoin, J. L., Gervais, F., Quittet, A. M. & Luspin, Y. Infrared and Raman responses in ferroelectric perovskite crystals: apparent inconsistencies. Phys. Rev. B 21, 2038–2041 (1980).
Huang, Z. et al. Temperature dependence of BaTiO3 infrared dielectric properties. Appl. Phys. Lett. 88, 212902 (2006).
Ashcroft, N. W. & Mermin, N. D. Solid State Physics Vol. 848 (Cengage Learning, 1976).
Kinsey, N., DeVault, C., Boltasseva, A. & Shalaev, V. M. Near-zero-index materials for photonics. Nat Rev Mater 4, 742–760 (2019).
Alam, M. Z., De Leon, I. & Boyd, R. W. Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region. Science 352, 795–797 (2016).
Smith, D. R., Pendry, J. B. & Wiltshire, M. C. K. Metamaterials and negative refractive index. Science 305, 788–792 (2004).
Reshef, O., De Leon, I., Alam, M. Z. & Boyd, R. W. Nonlinear optical effects in epsilon-near-zero media. Nat Rev Mater 4, 535–551 (2019).
Murdin, B. N. Far-infrared free-electron lasers and their applications. Contemp. Phys. 50, 391 (2009).
Jaroszynski, D. A. et al. Experimental observation of limit-cycle oscillations in a short-pulse free-electron laser. Phys. Rev. Lett. 70, 3412–3415 (1993).
Janssen, T. et al. Cavity-dumping a single infrared pulse from a free-electron laser for two-color pump-probe experiments. Rev. Sci. Instrum. 93, 043007 (2022).
Liberal, I. & Engheta, N. Near-zero refractive index photonics. Nat. Photon. 11, 149–158 (2017).
Kinsey, N. & Khurgin, J. Nonlinear epsilon-near-zero materials explained: opinion. Opt. Mater. Express 9, 2793–2796 (2019).
Fahy, S. & Merlin, R. Reversal of ferroelectric domains by ultrashort optical pulses. Phys. Rev. Lett. 73, 1122–1125 (1994).
Subedi, A. Proposal for ultrafast switching of ferroelectrics using midinfrared pulses. Phys. Rev. B 92, 214303 (2015).
Subedi, A., Cavalleri, A. & Georges, A. Theory of nonlinear phononics for coherent light control of solids. Phys. Rev. B 89, 220301 (2014).
Mankowsky, R., von Hoegen, A., Först, M. & Cavalleri, A. Ultrafast reversal of the ferroelectric polarization. Phys. Rev. Lett. 118, 197601 (2017).
Ciattoni, A. et al. Enhanced nonlinear effects in pulse propagation through epsilon-near-zero media. Laser Photon. Rev. 10, 517–525 (2016).
Xu, Z. & Arnoldus, H. F. Reflection by and transmission through an ENZ interface. OSA Continuum 2, 722–735 (2019).
Arnoldus, H. F. Penetration of dipole radiation into an ENZ medium. Opt. Commun. 489, 126867 (2021).
Khalsa, G., Benedek, N. A. & Moses, J. Ultrafast control of material optical properties via the infrared resonant Raman effect. Phys. Rev. X 11, 021067 (2021).
Stupakiewicz, A. et al. Ultrafast phononic switching of magnetization. Nat. Phys. 17, 489–492 (2021).
Stremoukhov, P. et al. Phononic manipulation of antiferromagnetic domains in NiO. New J. Phys. 24, 023009 (2022).
Sones, C. L. et al. Ultraviolet laser-induced sub-micron periodic domain formation in congruent undoped lithium niobate crystals. Appl. Phys. B 80, 341–344 (2005).
Steigerwald, H. et al. Direct writing of ferroelectric domains on the x-and y-faces of lithium niobate using a continuous wave ultraviolet laser. Appl. Phys. Lett. 98, 062902 (2011).
Xu, X. et al. Femtosecond laser writing of lithium niobate ferroelectric nanodomains. Nature 609, 496–501 (2022).
Yang, M.-M. & Alexe, M. Light-induced reversible control of ferroelectric polarization in BiFeO3. Adv. Mater. 30, 1704908 (2018).
Back, C. H. et al. Magnetization reversal in ultrashort magnetic field pulses. Phys. Rev. Lett. 81, 3251 (1998).
Vlasov, V. S. et al. Magnetization switching in bistable nanomagnets by picosecond pulses of surface acoustic waves. Phys. Rev. B 101, 024425 (2020).
Denev, S. A. et al. Probing ferroelectrics using optical second harmonic generation. J. Am. Ceram. Soc. 94, 2699–2727 (2011).
Uesu, Y., Kurimura, S. & Yamamoto, Y. Optical second harmonic images of 90° domain structure in BaTiO3 and periodically inverted antiparallel domains in LiTaO3. Appl. Phys. Lett. 66, 2165–2167 (1995).
Zgonik, M. et al. Dielectric, elastic, piezoelectric, electro-optic, and elasto-optic tensors of BaTiO3 crystals. Phys. Rev. B 50, 5941–5949 (1994).
Acknowledgements
We acknowledge A.K. Tagantsev for useful discussions and thank the technical staff at FELIX for providing technical support. We thank J. van Eeten for his experimental contributions. D.G.L. acknowledges funding by the Max Planck–Radboud University Center for Infrared Free Electron Laser Spectroscopy. A.K., M.K. and C.S.D. acknowledge funding by the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (Netherlands Organisation for Scientific Research). C.S.D. acknowledges support from the European Research Council ERC grant agreement no. 101115234 (HandShake).
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A.K. conceived the project. M.K. and D.G.L. performed the measurements. C.S.D. assisted in building the experimental set-up. A.K, M.K and C.S.D. wrote the paper. All authors were involved in discussing the results.
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Nature Photonics thanks Roman Mankowsky, Vasily Temnov and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Discussion 1–7, Figs. 1–9 and References.
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Raw data of images used in Fig. 1; Fig. 2 data points of switching lengths used in graph; and code to calculate electric displacement field shown in Fig. 3c.
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Kwaaitaal, M., Lourens, D.G., Davies, C.S. et al. Epsilon-near-zero regime enables permanent ultrafast all-optical reversal of ferroelectric polarization. Nat. Photon. (2024). https://doi.org/10.1038/s41566-024-01420-3
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DOI: https://doi.org/10.1038/s41566-024-01420-3