Abstract
Nanomaterials with a large chiroptical response and high structural stability are desirable for advanced miniaturized optical and optoelectronic applications. One-dimensional (1D) nanotubes are robust crystals with inherent and continuously tunable chiral geometries. However, their chiroptical response is typically weak and hard to control, due to the diverse structures of the coaxial tubes. Here we demonstrate that as-grown multiwalled boron nitride nanotubes (BNNTs), featuring coherent-stacking structures including near monochirality, homo-handedness and unipolarity among the component tubes, exhibit a scalable nonlinear chiroptical response. This intrinsic architecture produces a strong nonlinear optical response in individual multiwalled BNNTs, enabling second-harmonic generation (SHG) with a conversion efficiency up to 0.01% and output power at the microwatt level—both excellent figures of merit in the 1D nanomaterials family. We further show that the rich chirality of the nanotubes introduces a controllable nonlinear geometric phase, producing a chirality-dependent SHG circular dichroism with values of −0.7 to +0.7. We envision that our 1D chiral platform will enable novel functions in compact nonlinear light sources and modulators.
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Data availability
The data supporting the findings of this study are presented within the paper and Supplementary Information. Additional data are available from the corresponding authors upon reasonable request. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Key R&D Program of China (2022YFA1403504 (K.L.)), National Natural Science Foundation of China (52025023 (K.L.), 12374167 (H.H.), 51991342 (K.L.), 62305003 (Chaojie Ma) and 92163206 (M.W.)), Guangdong Major Project of Basic and Applied Basic Research (2021B0301030002 (E.W. and K.L.)), Strategic Priority Research Program of Chinese Academy of Sciences (XDB33000000 (K.L.)), China Postdoctoral Science Foundation (2022M710232 (C.L.)) and New Cornerstone Science Foundation through the XPLORER PRIZE (K.L.).
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K.L. and H.H. supervised and conceived the projects. Chaojie Ma and C.L. performed the SHG and HHG experiments. Chaojie Ma and Chenjun Ma performed the chiroptical measurement. Chenjun Ma, H.H., C.H., J.L. and Z.S. contributed the theoretical calculations. Q.G., M.W., P.G. and X.B. conducted the TEM experiments. M.L., X.S. and W.W. prepared and processed BNNT samples. Q.G., J.Q. and B.Q. conducted the scanning electron microscopy and atomic force microscopy measurements. G.Y., Z.S. and E.W. suggested the optical experiments. All the authors discussed and contributed to writing the paper.
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Nature Nanotechnology thanks Qinwei An, Shengxi Huang and Enrique Diez for their contribution to the peer review of this work.
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Ma, C., Ma, C., Liu, C. et al. Strong chiroptical nonlinearity in coherently stacked boron nitride nanotubes. Nat. Nanotechnol. (2024). https://doi.org/10.1038/s41565-024-01685-3
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DOI: https://doi.org/10.1038/s41565-024-01685-3
