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Layered hybrid superlattices with a regulated intersystem crossing process

Nature Synthesis volume 5, pages 272–280 (2026)Cite this article

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Abstract

Layered organic–inorganic hybrid superlattices, with modular structural advantages, offer an interesting approach to overcome the challenges in modulating the efficiency of intersystem crossing (ISC). This hybrid material system integrates the variable electronic and atomic properties of inorganic metal layers with the programmable chemical properties of organic coordination layers, enabling regulation of electronic states, excitons and ISC processes. Here we demonstrate a precise ISC modulating strategy by constructing gold-based organic–inorganic layered hybrid superlattices, featuring alternately assembled atomically thin gold layers and 4-mercapto-benzamide-derived organic ligands layers. The confined layered structure achieves directional hybridization between transition metal d orbitals and delocalized electrons of organic moieties through controlled Au–π conjugation interactions. Femtosecond transient-absorption spectroscopy reveals that ISC time decreases from >2 ps to 0.26 ps as interlayer spacing reduces, demonstrating the role of structural confinement in promoting ultrafast ISC. Moreover, temperature-dependent photoluminescence studies estimate the singlet–triplet energy gap at ∼20 meV, further supporting the enhanced ISC mechanism. This work introduces the design of hybrid superlattices with tailored spin–orbit interactions enabling tunable fluorescence and phosphorescence properties, paving the way for next-generation optoelectronic applications.

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Fig. 1: Synthesis and characterization of Au-LHSLs.
Fig. 2: Structure characterization of various Au-LHSLs.
Fig. 3: Luminescent properties of Au-LHSLs.
Fig. 4: Ultrafast excited-state dynamics results of Au-LHSLs.
Fig. 5: Charge redistribution induced by layered hybrid superlattice structure.

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All data are available in the main text or the Supplementary Information.

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Acknowledgements

We acknowledge the support of the NSRL in the XAFS experiments. We are grateful to the Analysis & Testing Center of Beihang University for the facilities, and for scientific and technical assistance. We are grateful for support from the National Natural Science Foundation of China (52572197, T.G.; 51532001, L.G.; 52522315, P.H.; 52371147, P.H.), the National Key Research and Development Program (2023YFA1507002, X.L.), the Strategic Priority Research Program of Chinese Academy of Sciences (XDB0770000, X.L.), the National Science Foundation for Distinguished Young Scholars of China (22325301, X.L.), the Fundamental Research Funds for the Central Universities (JKF-20240451 and YWF-23-L-1232, P. H.). T.G. thanks the National Natural Science Foundation of China for Excellent Young Scientists (Overseas) for support.

Author information

Author notes

  1. These authors contributed equally: Haosen Yang, Yutong Zhang, Zhengyao Qiu, Hongfei Gu.

Authors and Affiliations

  1. State Key Laboratory of Bioinspired Interfacial Materials Science, Bioinspired Science Innovation Center, Hangzhou International Innovation Institute, Beihang University, Hangzhou, China

    Haosen Yang, Hongfei Gu, He Guo & Lin Guo

  2. School of Chemistry, Beihang University, Beijing, China

    Haosen Yang, Hongfei Gu, He Guo, Pengfei Hu & Lin Guo

  3. CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, Beijing, China

    Yutong Zhang, Lingyun Zhu, Shuai Yue & Xinfeng Liu

  4. University of Chinese Academy of Sciences, Beijing, China

    Yutong Zhang, Lingyun Zhu, Shuai Yue & Xinfeng Liu

  5. Research Institute of Aero-Engine, Beihang University, Beijing, China

    Zhengyao Qiu & Pengfei Hu

  6. International Research Institute for Multidisciplinary Science, Beihang University, Beijing, China

    Tianqi Guo

Authors
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Contributions

L.G. conceived and led this project. H.Y. prepared the samples. P.H., T.G., H.Y., H. Guo and Z.Q. conducted characterizations and analysed the results. H. Gu conducted EXAFS tests and analysed the results. Y.Z., L.Z., S.Y. and X.L. conducted the fluorescence measurements and analysed the results. All authors participated in the discussion. L.G., P.H., H.Y., T.G. and X.L. analysed the data and co-wrote this paper.

Corresponding authors

Correspondence to Tianqi Guo, Pengfei Hu, Shuai Yue, Xinfeng Liu or Lin Guo.

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Nature Synthesis thanks Dongpeng Yan and the other, anonymous, reviewer(s) 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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Supplementary Figs. 1–19, Discussion and Tables 1–3.

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Ultrafast excited-state dynamics sources data

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Yang, H., Zhang, Y., Qiu, Z. et al. Layered hybrid superlattices with a regulated intersystem crossing process. Nat. Synth 5, 272–280 (2026). https://doi.org/10.1038/s44160-025-00921-5

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