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Synthesis of single-unit-cell-thick perovskites by liquid-phase confined assembly for high-performance ultrastable X-ray detectors

Nature Synthesis (2025)Cite this article

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Abstract

The instability of halide perovskites under working conditions or during complex postprocessing is challenging for practical applications. Here we developed a room-temperature, two-phase assembling strategy to synthesize single-unit-cell perovskite chains within single-walled carbon nanotubes (SWCNTs). This approach is efficient, scalable and tailorable, and can be used to assemble a range of single-chain perovskites. The single-unit-cell-chain perovskites show unconventional stoichiometries (such as [Cs4PbI5]+) due to dimensionality reduction and are balanced by negatively charged nanotubes. A direct X-ray detector constructed with high-entropy-Cs3MCl6@SWCNT exhibits outstanding performance, with a high sensitivity of \(1.22\times10^{4}\,\upmu{\mathrm{C}}\,{\mathrm{Gy}}_{\mathrm{air}}^{-1}\,{\mathrm{cm}}^{-2}\), a low dark current density of 0.2 nA cm−2, a negligible dark current drift of 8.5 × 10−7 nA cm−1 s−1 V−1 and a superior detection limit of 16.6 nGyair s−1. These surpass various common semiconductor and state-of-the-art perovskite detectors due to the ionic character of perovskite@SWCNT inducing a strong cation–π interaction, suppressing ion migration. The device is stable under harsh conditions, including continuous X-ray irradiation, high temperatures, exposure to ambient air for 91 days and immersion for 96 h in water. This low-cost synthetic methodology paves the way for the commercialization of potential perovskite X-ray detectors for medical and industrial applications.

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Fig. 1: Characterization of CsPbI3@SWCNT.
Fig. 2: Universal synthesis of ABX3 and AB2X3 perovskites within SWCNTs and BNNTs.
Fig. 3: Characterization of medium- and high-entropy Cs3MCl6@SWCNT.
Fig. 4: MD simulations.
Fig. 5: Doping of ABX3@SWCNT by solution-phase ion exchange.
Fig. 6: High-entropy Cs3MCl6@SWCNT-based direct X-ray detector.

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Data availability

All data that support this work are available within the paper and its Supplementary Information. Source data are provided with this paper. Crystallographic information files have also been deposited in the Inorganic Crystal Structure Database under reference numbers ICSD 161481, 201285, 29067, 177350, 28082, 131089, 262924, 241488, 68819, 53835, and in Material Project under reference numbers mp-27336 and mp-1112341. These data can be obtained free of charge via https://www.ccdc.cam.ac.uk/structures/ or https://next-gen.materialsproject.org/materials.

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Acknowledgements

We gratefully acknowledge Z. W. Quan and Y. Wei for valuable discussions and the Core Research Facilities of SUSTech for characterization. F.Y. acknowledges support from the National Natural Science Foundation of China (NSFC) (22222504, 22475093, 92161124, 92461307), the National Key Research and Development Program of China (2021YFA0717400), the Shenzhen Basic Research Project (JCYJ20210324104808022), the State Key Laboratory of Advanced Fiber Materials (Donghua University) (KF2504) and the Guangdong Pearl River Talent Plan (2021QN02C104). Y.L. acknowledges support from the NSFC (52203342, 62304236), the National Key Research and Development Program of China (2024YFF0507802), the Shenzhen Basic Research Project (JCYJ20240813155804007), the Young Elite Scientist Sponsorship Program by Cast of China Association for Science and Technology (YESS20210285) and the Guangdong Pearl River Talent Plan (2021QN02Y300). DFT calculations were performed with the CHEM high-performance supercomputer cluster (CHEM-HPC) located at Department of Chemistry, SUSTech.

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Author notes

  1. These authors contributed equally: Meihui Song, Bo Zhao.

Authors and Affiliations

  1. Department of Chemistry, Southern University of Science and Technology, Shenzhen, China

    Meihui Song, Bowen Li, Kun Wang, Yulong Jiang, Guodong Jia, Xin Zhao, Boyuan Yu & Feng Yang

  2. Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Bo Zhao & Yunlong Li

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  1. Meihui Song
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Contributions

F.Y. conceived the project. F.Y. and Y.L. co-supervised the project and led the collaboration efforts. M.S. performed material synthesis. M.S., K.W., Y.J., G.J., X.Z. and B.Y. performed the characterizations. B.L. performed theoretical calculations. B.Z. and Y.L. contributed to the devices. F.Y., M.S., Y.L. and B.Z. wrote and revised the manuscript. All authors analysed the data, discussed the results and approved the manuscript.

Corresponding authors

Correspondence to Yunlong Li or Feng Yang.

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F.Y. and M.S. declare a financial interest: a patent related to this research has been submitted. The remaining authors declare no competing financial interests.

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Nature Synthesis thanks Paul Sellin and Jeremy Sloan for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.

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Extended data

Extended Data Fig. 1 Evidence of negatively charged SWCNT after filling perovskite.

a, Density of states of CsPbI3@(20,0)-SWCNT and projected density of states of (20,0)-SWCNT and [Cs4PbI5]. Fermi levels of CsPbI3@(20,0)-SWCNT and empty (20,0)-SWCNT are labelled, which is calculated by HSE06 functional. b, Raman spectra showing G band of CsPbI3@SWCNT and empty-SWCNT. Excitation wavelength: 532 nm.

Source data

Extended Data Fig. 2 Resistance of devices measured in the dark condition.

a, Senary Cs3MCl6@SWCNT. b, CsPbBr3@SWCNT. c, CsPbI3@SWCNT.

Source data

Extended Data Fig. 3 Bias-dependent photocurrent of senary Cs3MCl6@SWCNT device.

A modified Hecht equation is used to fit the obtained photoconductivity curve by the equation: \(I=\frac{{I}_{0}\mu \tau V}{{L}^{2}}[1-\exp (-\frac{{L}^{2}}{\mu \tau V})]\) where I0 is the saturated photoinduced signal current, V is the applied bias, and L is the thickness of the sample.

Source data

Extended Data Fig. 4 Photocurrent and dark current drift.

I-t curves of senary Cs3MCl6@SWCNT device in the dark and irradiation conditions with a bias of 200 V.

Source data

Extended Data Fig. 5 Ion-migration activation energy.

a, Senary Cs3MCl6@SWCNT. b, CsPbBr3@SWCNT. c, CsPbI3@SWCNT.

Source data

Extended Data Fig. 6 LoD evaluation.

a, I-t curves of senary Cs3MCl6@SWCNT device under a pulsing X-ray irradiation with different dose rates. b, X-ray dose rate dependent signal-to-noise ratio for LoD evaluation.

Source data

Extended Data Fig. 7 Statistic box showing the reproducibility of senary Cs3MCl6@SWCNT devices.

a, Sensitivities obtained at 50–200 V biases. b, LoD obtained at 200 V bias. c, Dark current drift obtained at 200 V bias. d, Dark current obtained at the 200 V bias. The data in (a–d) are collected from 6 different devices (n = 6) fabricated by the same materials and procedures. The upper line of the whisker represents the maximum value of the group of data, the lower line of the whisker represents the minimum value of the group of data, the upper edge of the box is the 75% quantile of the group of data, the lower edge of the box is the 25% quantile of the group of data, the middle line of the box is the median of the group of data, the curve is the average normal distribution of the group of data, and the white square in the centre of the box represents the mean of the group of the data.

Source data

Extended Data Fig. 8 Long-term storage stability of the senary Cs3MCl6@SWCNT device.

Normalized current-time curves when exposing the device to ambient air for 91 days.

Source data

Supplementary information

Supplementary Information

Supplementary Methods, Figs. 1–26, Tables 1–10, References 1–17 and caption for Supplementary Video 1.

Reporting Summary

Supplementary Video 1

A real-time movie of molecular dynamic simulations showing the diffusion behaviours of DMSO and cyclohexane molecules inside a (18,0) SWCNT with a diameter of 14.2 Å in 100 ns. Frame rate of video: 30 frame·s–1.

Source data

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Song, M., Zhao, B., Li, B. et al. Synthesis of single-unit-cell-thick perovskites by liquid-phase confined assembly for high-performance ultrastable X-ray detectors. Nat. Synth (2025). https://doi.org/10.1038/s44160-025-00785-9

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