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Nanoscale subparticle imaging of vibrational dynamics using dark-field ultrafast transmission electron microscopy

Nature Nanotechnology volume 18, pages 145–152 (2023)Cite this article

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Abstract

An understanding of nanoscale energy transport and acoustic response is important for applications of nanomaterials but hinges on a complete characterization of their structural dynamics. The precise determination of the structural dynamics within nanoparticles, however, is still challenging and requires high spatiotemporal resolution and detection sensitivity. Here we present a centred dark-field imaging approach based on ultrafast transmission electron microscopy that is capable of directly mapping the picosecond-scale evolution of intrananoparticle vibration with a spatial resolution down to 3 nm. Using this approach, we investigated the photo-induced vibrational dynamics in individual gold heterodimers composed of a nanoprism and a nanosphere. We observed not only the retardation of in-plane vibrations in the nanoprisms, which we attribute to thermal and vibrational energy transferred from adjacent nanospheres mediated by surfactants, but also the existence of a complex multimodal oscillation and its spatial variation within individual nanoprisms. This work represents an advance in real-space mapping of vibrational dynamics on the subnanoparticle level with a high detection sensitivity.

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Fig. 1: Schematic of the UHS-CDF imaging setup and structural dynamics of isolated Au nanoprisms on various substrates.
Fig. 2: Overall structural dynamics of an Au nanoprism–nanosphere heterodimer on the Si3N4 substrate.
Fig. 3: Numerical simulation of thermal evolution in heterodimers.
Fig. 4: Intrananoparticle oscillation analysis of the Au nanoprism in the heterodimer on the Si3N4 substrate.
Fig. 5: Effect of structural deformation on vibrational interactions of Au nanoparticles on the Si3N4 substrate.

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Data availability

The data that support the findings of this study are available within the paper and the Supplementary Information. Other relevant data are available from the corresponding author upon reasonable request. Source data are provided with this paper.

Code availability

The codes that support the findings of this study are available from the corresponding author upon reasonable request.

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  • 19 December 2022

    In the version of this article initially published, the Supplementary Information file was incorrect and has been restored in the online version of the article.

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Acknowledgements

This research was supported by the National Natural Science Foundation of China (grant nos. 51571035 and 11774032). We thank D. S. Li, X. F. Kang and J. S. Baskin for their help in UTEM experiments, and P. Wang and S. Gao for their help in EELS experiments.

Author information

Authors and Affiliations

  1. Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Ling Tong, Zhiwei Zhang & Zhiwei Wang

  2. School of Nanoscience and Technology, University of Chinese Academy of Sciences, Beijing, People’s Republic of China

    Ling Tong, Zhiwei Zhang & Zhiwei Wang

  3. School of Physics, Engineering and Technology, University of York, York, UK

    Jun Yuan

  4. The Institute for Technological Sciences, Wuhan University, Wuhan, People’s Republic of China

    Jau Tang

  5. Center on Nanoenergy Research, School of Physical Science and Technology, Guangxi University, Nanning, People’s Republic of China

    Zhiwei Wang

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  1. Ling Tong
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Contributions

Z.W. conceived the research project. L.T. and Z.W. performed the UTEM experiments. L.T., Z.W. and J.T. conducted the UTEM data analysis. L.T., Z.Z., Z.W. and J.Y. carried out numerical simulation and analysis. All authors discussed the results. Z.W., L.T. and J.Y. wrote the manuscript with input and comments from all authors.

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Correspondence to Zhiwei Wang.

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The authors declare no competing interests.

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Nature Nanotechnology thanks Florian Banhart, David Flannigan and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Methods, Notes, Figs. 1–28 and Videos 1–6.

Supplementary Video 1

Experimentally acquired time-delay BF-UTEM image series and intensity analysis corresponding to Supplementary Fig. 5a,c.

Supplementary Video 2

Experimentally acquired time-delay UHS-CDF image series and intensity analysis corresponding to Supplementary Fig. 5b,d.

Supplementary Video 3

Simulated time-delay UHS-CDF image series and intensity analysis corresponding to Supplementary Fig. 6.

Supplementary Video 4

Simulated time-delay BF-UTEM image series and intensity analysis corresponding to Supplementary Fig. 7.

Supplementary Video 5

Experimentally acquired time-delay UHS-CDF image series and intensity analysis corresponding to Fig. 2d.

Supplementary Video 6

Intrananoprism frequency evolution corresponding to Fig. 4d. The oscillation frequency was measured from a square region of 10 nm wide, whose centre is marked with the red dot. The selected region shifts laterally and pixel by pixel (pixel size, 3.3 Å).

Source data

Source Data Fig. 1

Statistical source data for Fig. 1b,c.

Source Data Fig. 2

Statistical source data for Fig. 2d.

Source Data Fig. 3

Statistical source data for Fig. 3a,b.

Source Data Fig. 4

Statistical source data for Fig. 4c.

Source Data Fig. 5

Statistical source data for Fig. 5d.

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Tong, L., Yuan, J., Zhang, Z. et al. Nanoscale subparticle imaging of vibrational dynamics using dark-field ultrafast transmission electron microscopy. Nat. Nanotechnol. 18, 145–152 (2023). https://doi.org/10.1038/s41565-022-01255-5

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