Abstract
Recent breakthroughs in ultrathin, single-crystalline, freestanding complex oxide systems have sparked industry interest in their potential for next-generation commercial devices1,2. However, the mass production of these ultrathin complex oxide membranes has been hindered by the challenging requirement of inserting an artificial release layer between the epilayers and substrates3,4. Here we introduce a technique that achieves atomic precision lift-off of ultrathin membranes without artificial release layers to facilitate the high-throughput production of scalable, ultrathin, freestanding perovskite systems. Leveraging both theoretical insights and empirical evidence, we have identified the pivotal role of lead in weakening the interface. This insight has led to the creation of a universal exfoliation strategy that enables the production of diverse ultrathin perovskite membranes less than 10 nm. Our pyroelectric membranes demonstrate a record-high pyroelectric coefficient of 1.76 × 10−2 C m−2 K−1, attributed to their exceptionally low thickness and freestanding nature. Moreover, this method offers an approach to manufacturing cooling-free detectors that can cover the full far-infrared spectrum, marking a notable advancement in detector technology5.
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Acknowledgements
This work was supported by the Air Force Office of the Scientific Research (AFOSR) (award no. FA9550−22-1-0024). C.B.E. acknowledges support for this research through a Vannevar Bush Faculty Fellowship (ONR N00014-20-1-2844) and the EPiQS Initiative of the Gordon and Betty Moore Foundation (grant no. GBMF9065). Ferroelectric measurement at the University of Wisconsin–Madison was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), under award no. DE-FG02-06ER46327. C.S.C. acknowledges support for this research by the NRF grant funded by the Korea Government (MSIT) (grant nos. RS-2024-00355333 and RS-2024-00451173). We thank J. A. del Alamo for providing access to the electrical characterization equipment in his laboratory.
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J.K. conceived the idea and directed the team. X. Zhang designed and coordinated the experiments and characterization. O.E., P.P. and S. Lindemann performed epitaxial growth by sputtering, under the guidance of C.B.E. X. Zhang performed growth by pulsed laser deposition. M.A. and Y.F.S. conducted simulations of heterostructures using DFT. X. Zhang, S. Lee, N.M.H. and H.K. developed the mechanical exfoliation theory. C.S.C. and H.L. performed and analysed the TEM measurements. X. Zhang, O.E., S. Lindemann, P.P. and Y. Shao conducted materials characterizations. Exfoliation and device fabrication were carried out by X. Zhang, J.M.S. and J.-E.R. X. Zhang set up a confocal optical path and conducted pyroelectric characterization. J.M.S. designed all schematic illustrations. S. Lee, M.-K.S., J.M.S., J.-E.R., X. Zheng, B.B., H.K. and H.S.K. provided feedback throughout experiments and data analysis. The paper was written by X. Zhang, S. Lee, M.-K.S., C.S.C., Y.F.S. and J.K. All authors contributed to the analysis and discussion of the results leading to the paper.
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Extended data figures and tables
Extended Data Fig. 1 Characterization of PMN-PT on NSO substrate.
a, TEM cross-section image of as-grown PMN-PT/NSO. b, Fast Fourier transform (FFT) patterns of a selected area of a including the PMN-PT epilayer (i), PMN-PT/NSO interface (ii) and NSO substrate (iii). The lattice direction of the pattern is labelled with the red rectangle. The in-plane lattice parameter for both PMN-PT film and NSO substrate is calculated as 4.158 A along the [010] direction, confirming coherent epitaxy. c, XRD Azimuthal φ scan of (101) PMN-PT after exfoliation and growth on NSO, confirming the maintained single crystallinity without in-plane rotation.
Extended Data Fig. 2 Result of charge transfer calculated by DFT simulations.
Charge transfer of PTO/STO (left) and BTO/STO (right) supercell by DFT calculation. In the three-dimensional structural plots, red and blue areas represent charge acceptance and donation, respectively. The two-dimensional maps present the visualized charge transfer at the A-face from the epilayer (top), the interface (middle) and the B-face from the substrate (bottom).
Extended Data Fig. 3 Theoretical guidelines for different Pb-containing heterostructures.
a-c, Different modes of peeling for PMN-PT/STO (a), PMN-PT/NSO (b), and PMN-PT/SRO (c) heterostructures as a function of Ni stressor thickness at an Ni stress level of 600 MPa. There is an exfoliation window with the change of stressor thickness for all three systems due to interface weakening, consistent with experiment observations.
Extended Data Fig. 4 Universal applicability of ALO to various Pb-based material systems.
a,b, Optical images (a) and EBSD maps (b) of exfoliated Pb-containing membrane with a size of 5 × 5 mm2, confirming high uniformity and maintained single crystallinity. c, Rocking curve of as-grown Pb-containing epilayers on different substrates. An FWHM ranging between 0.016° to 0.090° indicates good crystallinity of all epilayers. d,e, Optical images (d) and plan-view SEM (e) showing the surfaces of non-Pb-containing materials including BTO (left) and SRO (right) with spalled STO substrate layers. f, Peeling modes of heterostructure with different lattice mismatch. Exfoliation of Pb-containing materials occurs with lattice mismatches ranging from 2.9% to 0.026%. While non-Pb-containing materials with the same lattice mismatch shows spalling results, thus clearly substantiating the universal effect of Pb-related interface weakening. NSOa and NSOb refer to the two anisotropic in-plane pseudocubic lattice parameters of the NSO substrate.
Extended Data Fig. 5 Demonstration of universal applicability of ALO.
a, Schematic illustration of freestanding membrane production using PTO as an interlayer. b, Rocking curve of SRO epilayer grown on STO (left) and PTO-covered STO (right). The minimal difference in FWHM values indicates that the presence of the PTO interlayer does not affect the crystallinity of the top layer. c, Optical microscopic images (left) and photos (inset), EBSD maps (middle), and AFM images (right) of (i) STO/PTO and (ii) SRO/PTO, exfoliated from STO. The exfoliated films are around 5 × 5 mm2. The exfoliated surfaces show single crystallinity and root-mean-square (RMS) roughness of 0.34 nm and 0.19 nm for STO/PTO and SRO/PTO, respectively. d, AFM images of STO substrate surface after exfoliation with an RMS roughness of 0.14 nm and 0.20 nm. The substrate surface shows step terrace structures, which are consistent with that of the film, indicating precise crack propagation has occurred at the interface.
Extended Data Fig. 6 Production of large-scale 20 nm-thick membrane.
a, Optical microscopic image of an exfoliated film with a size of 10 × 10 mm2. b, Rocking curve of 20 nm-thick PMN-PT grown on STO with a FWHM of 0.283° indicating good crystallinity. c, EBSD maps with 4 × 4 positions over the entire membrane (top) and histograms showing misorientation angle distribution extracted from the maps (bottom). The misorientation angle distribution shows a peak position of 0.17° and a FWHM value of lower than 0.19°, confirming the maintained crystallinity on a large scale after exfoliation.
Extended Data Fig. 7 Characterization of PMN-PT on STO with various thicknesses.
a, 2 theta-omega XRD scans, and b, rocking curve of PMN-PT (002). XRD spectrums are shown for PMN-PT layers grown on STO substrate with thicknesses ranging between 10 to 200 nm. The vertical dashed line indicates the peak position for bulk PMN-PT. Good crystallinity is confirmed by the FWHM of the rocking curve ranging from 0.07° to 0.53°.
Extended Data Fig. 8 Reproducibility of ALO process.
a-d, Optical images (top left), AFM images (top right), EBSD maps (bottom right), and histograms showing misorientation angle distribution extracted from the maps (bottom left) of PMN-PT membranes exfoliated from STO with a thickness of 10 nm (a), 40 nm (b), 80 nm (c), and 200 nm (d) with a size of 5 × 5 mm. The RMS roughness of the surface ranges from 0.23 nm to 0.84 nm. The peak positions are all close to zero (0.09° to 0.25°) with a narrow width (0.09° to 0.54°), thus quantitatively indicating the preserved crystallinity and high uniformity after exfoliation.
Extended Data Fig. 9 Stability of pyroelectric response.
a, Average pyroelectric current density of 10 devices fabricated by PMN-PT membrane with a thickness of 10 nm under a temperature modulation frequency from 100 to 760 Hz. The error ribbon (coloured in light blue) presents their standard deviation. b, Pyroelectric current density of the device with a thickness of 10 nm under different temperature modulation amplitudes. The error ribbon (coloured in light blue) presents the standard deviation across 10 measurements. c, Pyroelectric current density recorded over time with a radiation modulation frequency of 760 Hz and amplitude of 4.6 K.
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Zhang, X., Ericksen, O., Lee, S. et al. Atomic lift-off of epitaxial membranes for cooling-free infrared detection. Nature 641, 98–105 (2025). https://doi.org/10.1038/s41586-025-08874-7
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DOI: https://doi.org/10.1038/s41586-025-08874-7
