Large electrocaloric effects in oxide multilayer capacitors over a wide temperature range

Abstract

Heat pumps based on magnetocaloric and electrocaloric working bodies—in which entropic phase transitions are driven by changes of magnetic and electric field, respectively—use displaceable fluids to establish relatively large temperature spans between loads to be cooled and heat sinks1,2. However, the performance of prototypes is limited because practical magnetocaloric working bodies driven by permanent magnets3,4,5 and electrocaloric working bodies driven by voltage6,7,8,9,10,11,12,13,14,15,16 display temperature changes of less than 3 kelvin. Here we show that high-quality multilayer capacitors of PbSc0.5Ta0.5O3 display large electrocaloric effects over a wide range of starting temperatures when the first-order ferroelectric phase transition is driven supercritically (as verified by Landau theory) above the Curie temperature of 290 kelvin by electric fields of 29.0 volts per micrometre. Changes of temperature in the large central area of the capacitor peak at 5.5 kelvin near room temperature and exceed 3 kelvin for starting temperatures that span 176 kelvin (complete thermalization would reduce these values from 5.5 to 3.3 kelvin and from 176 to 73 kelvin). If magnetocaloric working bodies were to be replaced with multilayer capacitors of PbSc0.5Ta0.5O3, then the established design principles behind magnetocaloric heat pumps could be repurposed for better performance without bulky and expensive permanent magnets.

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Fig. 1: MLC structure.
Fig. 2: Indirect EC measurements.
Fig. 3: Direct EC measurements.
Fig. 4: Large EC effects over a wide range of operating temperatures.

Data availability

Source data for Figs. 24 are provided with the paper. All other relevant data are available within the paper and its Supplementary Information files.

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Acknowledgements

We thank C. Minami, Y. Kojima, N. Furusawa, K. Yamamoto, Y. Inoue and K. Honda for their assistance in fabricating MLCs, and we thank R. Whatmore, À. Torelló and E. Defay for discussions. B.N. is grateful for support from Gates Cambridge, the Winton Programme for the Physics of Sustainability, and Trinity College Cambridge. X.M. is grateful for support from UK EPSRC grant EP/M003752/1, ERC starting grant no. 680032, and the Royal Society. G.G.G.-V. is grateful for support from the Vice-Rectory for Research (project no. B9194) and the Office of International Affairs at the University of Costa Rica, and Churchill College at the University of Cambridge. X.M. and G.G.G.-V. are grateful for support from the Royal Society International Exchanges programme (IES\R3\170025).

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N.D.M. and X.M. conceived the study and led the project together with B.N. and S.H. T.U. and S.H. were responsible for the fabrication and optimization of the high-quality MLCs. S.C. constructed and commissioned the bespoke apparatus used for electrical and thermal measurements. B.N. performed all of the measurements, except that S.K. performed the X-ray diffraction and obtained the optical images. G.G.G.-V. performed the Landau theory. N.D.M wrote the manuscript and supplementary file, with input and feedback from B.N., X.M., S.H., S.C. and G.G.G.-V.

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Correspondence to X. Moya or S. Hirose or N. D. Mathur.

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Peer review information Nature thanks Brahim Dkhil, Bai-Xiang Xu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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.This file contains Supplementary Notes 1-17 and References

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Nair, B., Usui, T., Crossley, S. et al. Large electrocaloric effects in oxide multilayer capacitors over a wide temperature range. Nature 575, 468–472 (2019). https://doi.org/10.1038/s41586-019-1634-0

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