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Aluminum nanocrystals evolving from cluster to metallic state: Size tunability and spectral evidence

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Abstract

Sub-3 nm aluminum (Al) nanocrystal is an emerging class of nanomaterial with properties distinct to noble metal nanoclusters. The complete solution synthesis of aluminum nanoclusters was recently reported, and their photoluminescence (PL) observed for the first time. At the moment, there exists no method to tune the size of ultrasmall aluminum nanocrystals in solution thus no knowledge on the boundary state between aluminum nanoclusters to plasmonic nanoparticles. In this work, it is demonstrated a study of size-controlled solution synthesis of ultrasmall aluminum nanocrystals with size controlled between ∼ 2.2 to ∼ 3.8 nm. Increasing the size results in three sets of spectral responses: (1) absorption due to nascent plasmons generated at ∼ 340 nm for larger particles, confirmed by Mie theory calculations; (2) significant decreased quantum yield of PL from ∼ 7.8% to ∼ 2.4%, indicating reduced quantum confinement effects and increased metallicity; (3) drop of fluorescence lifetime was observed, especially when the diameter of aluminum nanoparticles was changed from ∼ 3.0 to ∼ 3.8 nm. This study provides experimental evidence and insights to the transitional state between aluminum nanoclusters to plasmonic nanoparticles, which seems to occur at size larger than gold nanoclusters.

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Acknowledgements

We gratefully acknowledge the National Natural Science Foundation of China (Nos. 61905211, 91833303, 11621101, and 61774131), the National Key Research and Development Program of China (No. 2017YFA0205700), Science Foundation of Zhejiang Province (No. Y21B050009), the Fundamental Research Funds for the Central Universities (Nos. 511308*172210191 and 2019FZA5002), and Ningbo Science and Technology Project (No. 2018B10093). We wish to thank Prof. Y. Jin of College of Optical Science and Engineering, Zhejiang University, for valuable discussions on FDTD simulations.

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Authors and Affiliations

  1. National Engineering Research Centre for Optical Instruments, College of Optical Science and Engineering, Zhejiang University, Hangzhou, 310058, China

    Hao Wu, Xiaoyu Cheng, Hongguang Dong & Sailing He

  2. Ningbo Research Institute, Ningbo, 315100, China

    Xiaoyu Cheng, Songjun Xie & Sailing He

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  1. Hao Wu
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Correspondence to Xiaoyu Cheng or Sailing He.

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Wu, H., Cheng, X., Dong, H. et al. Aluminum nanocrystals evolving from cluster to metallic state: Size tunability and spectral evidence. Nano Res. 15, 838–844 (2022). https://doi.org/10.1007/s12274-021-3486-9

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