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Rapid growth of inch-sized lanthanide oxychloride single crystals

Nature Materials volume 24, pages 852–860 (2025)Cite this article

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Abstract

The layered lanthanide oxychloride (LnOCl) family, featuring a low equivalent oxide thickness, high breakdown field and magnetic ordering properties, holds great promise for next-generation van der Waals devices. However, the exploitation of LnOCl materials has been hindered by a lack of reliable methods for growing their single-crystalline phases. Here we achieved the growth of inch-sized bulk LnOCl single crystals and single-crystalline thin films with thickness down to the monolayer in a few hours. The monolayer LnOCl exhibits ultralow equivalent oxide thicknesses, for instance, LaOCl and SmOCl have values of 0.25 and 0.34, respectively. Furthermore, using LnOCl as a dielectric in graphene devices, we demonstrate wafer-scale enhancement of carrier mobility and a well-developed quantum Hall effect. The induced strong magnetic proximity effect by SmOCl and DyOCl enables efficient interfacial charge transfer with magnetic exchange coupling This work provides a general strategy for synthesizing large-sized single-crystalline layered materials, enriching the library of ultralow-equivalent-oxide-thickness dielectric materials, and two-dimensional magnetic materials with induced strong magnetic proximity effect.

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Fig. 1: Oriented attachment assisted by KCl flux.
Fig. 2: Preparation and exfoliation of LnOCl bulk single crystals.
Fig. 3: CVD growth of single-crystalline LnOCl (Ln = La and Sm) wafers and their dielectric properties.
Fig. 4: Transport characterization, ZSHE and MPE of SmOCl–graphene heterostructure devices.

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Data supporting the results of this study are provided in this Article and its Supplementary Information and are available from the corresponding authors upon request. Source data are provided with this paper.

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Acknowledgements

We thank Z. Liu and K. Jia for synthesizing graphene single-crystalline wafers, and H. Peng for discussions. This work was financially supported by the National Key Research and Development Program of China (no. 2022YFA1204900). This work is also supported by the National Key Research and Development Program of China (no. 2024YFE0202200), the National Science Foundation of China (nos. 52372038, 12374035 and T2188101) and the Innovation Program for Quantum Science and Technology (grant no. 2021ZD0302600). We acknowledge the Molecular Materials and Nanofabrication Laboratory (MMNL) in the College of Chemistry and Peking Nanofab at Peking University for the use of instruments. K.S.N. acknowledges support from the Ministry of Education, Singapore (Research Centre of Excellence award to the Institute for Functional Intelligent Materials (I-FIM), project no. EDUNC-33-18-279-V12), and from the Royal Society (UK, grant no. RSRP/R/190000). We thank the Materials Processing and Analysis Center, Peking University, for optical characterization.

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Author notes

  1. These authors contributed equally: Zhuofeng Shi, Wei Guo, Saiyu Bu, Lingmiao Ma.

Authors and Affiliations

  1. School of Materials Science and Engineering, Peking University, Beijing, People’s Republic of China

    Zhuofeng Shi, Saiyu Bu, Zhaoning Hu, Yaqi Zhu, Haotian Wu, Xiaohui Chen & Li Lin

  2. College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, People’s Republic of China

    Zhuofeng Shi, Yaqi Zhu & Xiaodong Zhang

  3. Key Laboratory for the Physics and Chemistry of Nanodevices and Center for Carbon-based Electronics, School of Electronics, Peking University, Beijing, People’s Republic of China

    Wei Guo & Ning Kang

  4. Center for Nanochemistry, Beijing National Laboratory for Molecular Science, College of Chemistry and Molecular Engineering, Peking University, Beijing, People’s Republic of China

    Lingmiao Ma & Li Lin

  5. Academy for Advanced Interdisciplinary Studies, Peking University, Beijing, People’s Republic of China

    Lingmiao Ma & Li Lin

  6. Institute for Functional Intelligent Materials, National University of Singapore, Singapore, Singapore

    Kostya S. Novoselov

  7. Department of Engineering, University of Cambridge, Cambridge, UK

    Boyang Mao

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Contributions

L.L. and N.K. conceived the experiment. L.L., N.K. and B.M. supervised the project. Z.S., L.M., H.W. and Z.H. conducted the crystal growth of MOCl. Z.S., L.M. and X.C. conducted the mechanical exfoliation of MOCl. Z.S., L.M., Z.H., X.Z. and Y.Z. obtained and analysed the OM, XPS, TEM, EDS, Raman and AFM data. W.G. and Z.S. conducted the MOCl/graphene device fabrication and electrical measurements. Z.S. conducted the MIM structure and took the measurements. S.B. carried out the theoretical calculations. The manuscript was written by L.L., N.K. and B.M. All authors discussed the results and wrote the manuscript.

Corresponding authors

Correspondence to Boyang Mao, Ning Kang or Li Lin.

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Nature Materials thanks Changgu Lee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–33, captions for Supplementary Videos 1–3 and Tables 1–4.

Supplementary Video 1 (download MP4 )

In situ OM observation of growth process_1.

Supplementary Video 2 (download MP4 )

In situ OM observation of growth process_2.

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In situ OM observation of growth process_3.

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Statistical source data.

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Shi, Z., Guo, W., Bu, S. et al. Rapid growth of inch-sized lanthanide oxychloride single crystals. Nat. Mater. 24, 852–860 (2025). https://doi.org/10.1038/s41563-025-02142-9

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