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Published July 19, 2018 | Supplemental Material
Journal Article Open

Direct Visualization of Photomorphic Reaction Dynamics of Plasmonic Nanoparticles in Liquid by Four-Dimensional Electron Microscopy

Abstract

Liquid-cell electron microscopy (LC-EM) provides a unique approach for in situ imaging of morphology changes of nanocrystals in liquids under electron beam irradiation. However, nanoscale real-time imaging of chemical and physical reaction processes in liquids under optical stimulus is still challenging. Here, we report direct observation of photomorphic reaction dynamics of gold nanoparticles (AuNPs) in water by liquid-cell four-dimensional electron microscopy (4D-EM) with high spatiotemporal resolution. The photoinduced agglomeration, coalescence, and fusion dynamics of AuNPs at different temperatures are studied. At low laser fluences, the AuNPs show a continuous aggregation in several seconds, and the aggregate size decreases with increasing fluence. At higher fluences close to the melting threshold of AuNPs, the aggregates further coalesced into nanoplates. While at fluences far above the melting threshold, the aggregates fully fuse into bigger NPs, which is completed within tens of nanoseconds. This liquid-cell 4D-EM would also permit study of other numerical physical and chemical reaction processes in their native environments.

Additional Information

© 2018 American Chemical Society. Received: April 29, 2018; Accepted: July 5, 2018; Published: July 5, 2018. This work was partially supported by the Air Force Office of Scientific Research Grant FA9550-11-1-0055S for research conducted in The Gordon and Betty Moore Center for Physical Biology at California Institute of Technology, and the National Key Research and Development Program of China (No. 2016YFA0300802) and NSFC (No. 11234001). We would like to thank J. S. Baskin and Mohammed Th. Hassan for help on setting the femtosecond laser system. We thank Mohammed Th. Hassan for help on PINEM measurement. We also wish to thank J. Tang for fruitful discussion. Author Contributions: A.H.Z. and X.F. proposed and designed the project; X.F., B.C., and C.L. performed the experiment; X.F. and B.C. analyzed the experimental data; all authors contributed to the discussion and writing of the manuscript. The authors declare no competing financial interest.

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August 19, 2023
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