Abstract
Creating chirality in achiral graphene and other two-dimensional materials has attracted broad scientific interest due to their potential application in advanced optics, electronics and spintronics. However, investigations into their optical activities and related chiro-electronic properties are constrained by experimental challenges, particularly in the precise control over the chirality of these materials. Here a universal wax-aided immersion method is developed to yield graphene rolls with controllable chiral angles, and the method can be generalized in other two-dimensional materials for high-yield fabrication. The left-handed and right-handed rolls exhibit optical activity and excellent spin selectivity effects with a spin polarization over 90% at room temperature. The discovery of tunable chirality-induced spin selectivity in tailored roll-shaped allotropes, achievable only through precise control of chirality, distinguishes itself from other carbon materials or existing chiral materials. Our Dirac fermion model shows that the electrons moving predominately along one side of the chiral roll develop a preferred spin polarization, and the rolling-chirality-induced spin selectivity is a result of this finite spin selectivity effect. Our method opens up opportunities for endowing achiral two-dimensional materials with tunable chirality, and may enable the emergence of quantum behaviours and room-temperature spintronic technologies.
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Acknowledgements
W.H. was supported by the National Key Research and Development Program (2022YFB3603800), National Natural Science Foundation of China (52121002, U21A6002 and T2441002) and Haihe Laboratory of Sustainable Chemical Transformations. Y. Shen was supported by the National Natural Science Foundation of China (22375141, 51473116 and 51103094). Xiaopeng Li was supported by the National Key Research and Development Program (2021YFA1400900) and National Natural Science Foundation of China (11934002). X.G. was supported by the National Natural Science Foundation of China (22275042). Q.L. was supported by the National Natural Science Foundation of China (22174098). S.D. was supported by the National Key Research and Development Program (2024YFA1209600) and National Natural Science Foundation of China (52373250 and 52003190). S.L. was supported by the National Natural Science Foundation of China (52073208 and 52473319). We thank J. Qu for discussions on the experiment of the fabrication of graphene rolls. We thank H. Ren and W. Gao for their assistance in device fabrication. Xiaopeng Li acknowledges encouraging discussions with X. Xie.
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Y. Shen, S.L. and W.H. conceived the idea and designed the experiments. E.Z. fabricated the graphene rolls; conducted the characterizations, ROA test and mCP-AFM tests; analysed the data; and participated in writing the manuscript. S.D. designed the CISS characterization, made the magnetoresistance test, took part in the mechanistic discussions and revised the manuscript. Xiaopeng Li provided a theoretical model for the electronic transport and participated in writing the manuscript. X.M. and Q.L. constructed the Raman spectrometer and performed the ROA test. X.G. participated in writing the manuscript and took part in the mechanistic discussions. L.L. conducted the mCP-AFM tests. S.C. helped in developing the graphene roll fabrication process. G.F. and Y. Song participated in the TEM analysis. Xiaojuan Li and Y.X. assisted in the fabrication of graphene rolls. Z.W. and K.X. contributed to transverse spin-valve device fabrication or analysis. X. Liu and X.Z. contributed to the second harmonic generation test of the chiral graphene roll. R.Z. and Q.J. contributed to single-walled carbon nanotube fabrication. W.M., Y.Z., Q.Z., B.W., J.L., J.Y. and Y.Y. participated in writing and editing the manuscript. W.H., Q.L., Y. Shen and S.L. supervised the project and edited the manuscript. All the authors took part in the discussion and writing.
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Nature Materials thanks Xinliang Feng, Kian Ping Loh and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Zhang, E., Ding, S., Li, X. et al. Graphene rolls with tunable chirality. Nat. Mater. 24, 377–383 (2025). https://doi.org/10.1038/s41563-025-02127-8
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DOI: https://doi.org/10.1038/s41563-025-02127-8
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