The ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals1,2,3,4,5, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality6,7,8,9 and emergent phenomena, as seen in perovskite heterostructures10,11,12. However, separation of these layers from the growth substrate has proved challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general method to create freestanding perovskite membranes. The key is the epitaxial growth of water-soluble Sr3Al2O6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr3Al2O6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds13,14.
Subscribe to Journal
Get full journal access for 1 year
only $4.92 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
Novoselov, K. S. et al. Electric field effect in atomically thin carbon films. Science 306, 666–669 (2004).
Dean, C. R. et al. Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices. Nature 497, 598–602 (2013).
Osada, M. & Sasaki, T. Two-dimensional dielectric nanosheets: novel nanoelectronics from nanocrystal building blocks. Adv. Mater. 24, 210–228 (2012).
Xu, M., Liang, T., Shi, M. & Chen, H. Graphene-like two-dimensional materials. Chem. Rev. 113, 3766–3798 (2013).
Butler, S. Z. et al. Progress, challenges, and opportunities in two-dimensional materials beyond graphene. ACS Nano 7, 2898–2926 (2013).
Wang, Q.-Y. et al. Interface-induced high-temperature superconductivity in single unit-cell FeSe films on SrTiO3 . Chin. Phys. Lett. 29, 037402 (2012).
Chang, C. Z. et al. Experimental observation of the quantum anomalous Hall effect in a magnetic topological insulator. Science 340, 167–170 (2013).
Shishido, H. et al. Tuning the dimensionality of the heavy fermion compound CeIn3 . Science 327, 980–983 (2010).
Bode, M. et al. Chiral magnetic order at surfaces driven by inversion asymmetry. Nature 447, 190–193 (2007).
Caviglia, A. D. Electric field control of the LaAlO3/SrTiO3 interface ground state. Nature 456, 624–627 (2008).
Mannhart, J. & Schlom, D. G. Oxide interfaces-an opportunity for electronics. Science 327, 1607–1611 (2010).
Hwang, H. Y. et al. Emergent phenomena at oxide interfaces. Nat. Mater. 11, 103–113 (2012).
Alferov, Z. I. Semiconductor Heterostructures: Physical Processes and Applications (MIR Publishers, 1989).
Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499, 419–425 (2013).
Bruel, M. Application of hydrogen ion beams to silicon on insulator material technology. Nucl. Instrum. Methods Phys. Res. Sect. B 108, 313–319 (1996).
Wong, W. S., Sands, T. & Cheung, N. W. Damage-free separation of GaN thin films from sapphire substrates. Appl. Phys. Lett. 72, 599–601 (1998).
Matthews, J. W. Growth of face-centered-cubic metals on sodium chloride substrates. J. Vac. Sci. Technol. 3, 133-145 (1966).
Catlin, A. & Walker, W. P. Mechanical properties of thin single-crystal gold films. J. App. Phys. 31, 2135–2139 (1960).
Rogers, J. A., Lagally, M. G. & Nuzzo, R. G. Synthesis, assembly and applications of semiconductor nanomembranes. Nature 477, 45–53 (2011).
Yablonovitch, E., Gmitter, T., Harbison, J. P. & Bhat, R. Extreme selectivity in the lift-off of epitaxial GaAs films. Appl. Phys. Lett. 51, 2222–2224 (1987).
Gan, Q., Rao, R. A., Eom, C. B., Garrett, J. L. & Lee, M. Direct measurement of strain effects on magnetic and electrical properties of epitaxial SrRuO3 thin films. Appl. Phys. Lett. 72, 978–980 (1998).
Paskiewicz, D. M., Sichel-Tissot, R., Karapetrova, E., Stan, L. & Fong, D. D. Single-crystalline SrRuO3 nanomembranes: a platform for flexible oxide electronics. Nano Lett. 16, 534–542 (2016).
Bullard, J. W. et al. Mechanisms of cement hydration. Cem. Concr. Res. 12, 1208–1223 (2011).
Alonso, J. A., Rasines, I. & Soubeyroux, J. L. Tristrontium dialuminum hexaoxide: an intricate superstructure of perovskite. Inorg. Chem. 29, 4768–4771 (1990).
Kim, K. S. et al. Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 457, 706–710 (2009).
Chen, X. et al. High-quality and efficient transfer of large area graphene films onto different substrates. Carbon 56, 271–278 (2013).
Kourkoutis, L. F., Song, J. H., Hwang, H. Y. & Muller, D. A. Microscopic origins for stabilizing room-temperature ferromagnetism in ultrathin manganite layers. Proc. Natl Acad. Sci. USA 107, 11682–11685 (2010).
Izumi, M., Ogimoto, Y., Manako, T., Kawasaki, M. & Tokura, Y. Interface effect and its doping dependence in La1−xSrxMnO3/SrTiO3 superlattices. J. Phys. Soc. Jpn 71, 2621–2624 (2002).
Thiele, C., Dorr, K., Bilani, O., Rodel, J. & Schultz, L. Influence of strain on the magnetization and magnetoelectric effect in La0.7A0.3MnO3/PMN-PT(001) (A = Sr, Ca). Phys. Rev. B 75, 054408 (2007).
Evans, A., Bieberle-Hütter, A., Rupp, J. L. M. & Gauckler, L. J. Review on microfabricated micro-solid oxide fuel cell membranes. J. Power Sources 194, 119–129 (2009).
Wang, Z. L. & Song, J. Piezoelectric nanogenerators based on zinc oxide nanowire arrays. Science 312, 242–246 (2006).
Ko, H. et al. Ultrathin compound semiconductor on insulator layers for high-performance nanoscale transistors. Nature 468, 286–289 (2010).
Nomura, K. et al. Room-temperature fabrication of transparent flexible thin-film transistors using amorphous oxide semiconductors. Nature 432, 488–492 (2004).
This work was supported by the Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under contract DE-AC02-76SF00515 (heterostructure synthesis); the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant GBMF4415 (development of release and transfer processes); and the Cornell Center for Materials Research with funding from the NSF MRSEC programme DMR-1120296 (electron microscopy).
The authors declare no competing financial interests.
About this article
Cite this article
Lu, D., Baek, D., Hong, S. et al. Synthesis of freestanding single-crystal perovskite films and heterostructures by etching of sacrificial water-soluble layers. Nature Mater 15, 1255–1260 (2016). https://doi.org/10.1038/nmat4749
Recent advances in development of magnetic garnet thin films for applications in spintronics and photonics
Journal of Alloys and Compounds (2021)
Nano-Micro Letters (2021)
Nano Letters (2021)
ACS Applied Materials & Interfaces (2021)
Epitaxial Stabilization and Oxygen Evolution Reaction Activity of Metastable Columbite Iridium Oxide
ACS Applied Energy Materials (2021)