Simultaneous manipulation of multiple boundary conditions in nanoscale heterostructures offers a versatile route to stabilizing unusual structures and emergent phases. Here, we show that a stable supercrystal phase comprising a three-dimensional ordering of nanoscale domains with tailored periodicities can be engineered in PbTiO3–SrRuO3 ferroelectric–metal superlattices. A combination of laboratory and synchrotron X-ray diffraction, piezoresponse force microscopy, scanning transmission electron microscopy and phase-field simulations reveals a complex hierarchical domain structure that forms to minimize the elastic and electrostatic energy. Large local deformations of the ferroelectric lattice are accommodated by periodic lattice modulations of the metallic SrRuO3 layers with curvatures up to 107 m−1. Our results show that multidomain ferroelectric systems can be exploited as versatile templates to induce large curvatures in correlated materials, and present a route for engineering correlated materials with modulated structural and electronic properties that can be controlled using electric fields.
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The STEM dataset and analysis used for calculating the curvature of the SrRuO3 layers can be found at temul-toolkit.readthedocs.io/en/latest/PTO_supercrystal_hadjimichael.html. Other datasets supporting the findings of this study are available from the corresponding authors upon reasonable request.
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We thank V. Tileli for preliminary TEM characterization and ESRF for provision of synchrotron radiation facilities. Parts of this work were supported by the EPSRC through grant nos. EP/M007073/1 (P.Z. and M.H.) and EP/S010769/1 (P.Z., Y.L. and E.Z.), the China Scholarship Council (Y.L.), UCL-ESRF Impact scholarship (E.Z.) and the A. G. Leventis Foundation (M.H.). J.H. and P.O. acknowledge support from the Czech Science Foundation (project 19-28594X). M.C., K.M., E.N.O’C. and U.B. acknowledge financial support from Science Foundation Ireland (SFI 16/US/3344). M.C. acknowledges funding from SFI Industry Fellowship (18/IF/6282).
The authors declare no competing interests.
Peer review information Nature Materials thanks Oleg Shpyrko and the other, anonymous, reviewers for their contribution to the peer review of this work.
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Hadjimichael, M., Li, Y., Zatterin, E. et al. Metal–ferroelectric supercrystals with periodically curved metallic layers. Nat. Mater. 20, 495–502 (2021). https://doi.org/10.1038/s41563-020-00864-6