3D Atomic-Scale Dynamics of Laser-Light-Induced Restructuring of Nanoparticles Unraveled by Electron Tomography

Wiebke Albrecht; Ece Arslan Irmak; Thomas Altantzis; Adrián Pedrazo-Tardajos; Alexander Skorikov; Tian Song Deng; Jessi E.S. van der Hoeven; Alfons van Blaaderen; Sandra Van Aert; Sara Bals

doi:10.1002/adma.202100972

3D Atomic-Scale Dynamics of Laser-Light-Induced Restructuring of Nanoparticles Unraveled by Electron Tomography

Wiebke Albrecht^*, Ece Arslan Irmak, Thomas Altantzis, Adrián Pedrazo-Tardajos, Alexander Skorikov, Tian Song Deng, Jessi E.S. van der Hoeven, Alfons van Blaaderen, Sandra Van Aert, Sara Bals

^*Corresponding author for this work

University of Antwerp

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Understanding light–matter interactions in nanomaterials is crucial for optoelectronic, photonic, and plasmonic applications. Specifically, metal nanoparticles (NPs) strongly interact with light and can undergo shape transformations, fragmentation and ablation upon (pulsed) laser excitation. Despite being vital for technological applications, experimental insight into the underlying atomistic processes is still lacking due to the complexity of such measurements. Herein, atomic resolution electron tomography is performed on the same mesoporous-silica-coated gold nanorod, before and after femtosecond laser irradiation, to assess the missing information. Combined with molecular dynamics (MD) simulations based on the experimentally determined 3D atomic-scale morphology, the complex atomistic rearrangements, causing shape deformations and defect generation, are unraveled. These rearrangements are simultaneously driven by surface diffusion, facet restructuring, and strain formation, and are influenced by subtleties in the atomic distribution at the surface.

Original language	English
Article number	2100972
Pages (from-to)	1-10
Number of pages	10
Journal	Advanced Materials
Volume	33
Issue number	33
DOIs	https://doi.org/10.1002/adma.202100972
Publication status	Published - 19 Aug 2021

Bibliographical note

Funding Information:
W.A. and E.A.I. contributed equally to this work. The authors acknowledge funding from the European Research Council under the European Union's Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 ‐ REALNANO and No. 770887 ‐ PICOMETRICS), the European Union's Seventh Framework Programme (ERC Advanced Grant No. 291667 ‐ HierarSACol), and the European Commission (EUSMI). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska‐Curie Actions (MSCA) in the Horizon 2020 program (Grant 797153, SOPMEN). T.‐S.D. acknowledges financial support from the National Science Foundation of China (NSFC, Grant No. 61905056). The authors also acknowledge financial support by the Research Foundation Flanders (FWO Grant G.0267.18N).

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Funding

W.A. and E.A.I. contributed equally to this work. The authors acknowledge funding from the European Research Council under the European Union's Horizon 2020 research and innovation program (ERC Consolidator Grants No. 815128 ‐ REALNANO and No. 770887 ‐ PICOMETRICS), the European Union's Seventh Framework Programme (ERC Advanced Grant No. 291667 ‐ HierarSACol), and the European Commission (EUSMI). W.A. acknowledges an Individual Fellowship funded by the Marie Sklodowska‐Curie Actions (MSCA) in the Horizon 2020 program (Grant 797153, SOPMEN). T.‐S.D. acknowledges financial support from the National Science Foundation of China (NSFC, Grant No. 61905056). The authors also acknowledge financial support by the Research Foundation Flanders (FWO Grant G.0267.18N).

Keywords

3D atomic structure
femtosecond laser excitation
gold nanorods
molecular dynamics
reshaping

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adma.202100972Final published version, 7.37 MBLicence: Taverne

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Albrecht, W., Arslan Irmak, E., Altantzis, T., Pedrazo-Tardajos, A., Skorikov, A., Deng, T. S., van der Hoeven, J. E. S., van Blaaderen, A., Van Aert, S., & Bals, S. (2021). 3D Atomic-Scale Dynamics of Laser-Light-Induced Restructuring of Nanoparticles Unraveled by Electron Tomography. Advanced Materials, 33(33), 1-10. Article 2100972. https://doi.org/10.1002/adma.202100972

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abstract = "Understanding light–matter interactions in nanomaterials is crucial for optoelectronic, photonic, and plasmonic applications. Specifically, metal nanoparticles (NPs) strongly interact with light and can undergo shape transformations, fragmentation and ablation upon (pulsed) laser excitation. Despite being vital for technological applications, experimental insight into the underlying atomistic processes is still lacking due to the complexity of such measurements. Herein, atomic resolution electron tomography is performed on the same mesoporous-silica-coated gold nanorod, before and after femtosecond laser irradiation, to assess the missing information. Combined with molecular dynamics (MD) simulations based on the experimentally determined 3D atomic-scale morphology, the complex atomistic rearrangements, causing shape deformations and defect generation, are unraveled. These rearrangements are simultaneously driven by surface diffusion, facet restructuring, and strain formation, and are influenced by subtleties in the atomic distribution at the surface.",

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AU - Pedrazo-Tardajos, Adrián

AU - Skorikov, Alexander

AU - Deng, Tian Song

AU - van der Hoeven, Jessi E.S.

AU - van Blaaderen, Alfons

AU - Van Aert, Sandra

AU - Bals, Sara

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AB - Understanding light–matter interactions in nanomaterials is crucial for optoelectronic, photonic, and plasmonic applications. Specifically, metal nanoparticles (NPs) strongly interact with light and can undergo shape transformations, fragmentation and ablation upon (pulsed) laser excitation. Despite being vital for technological applications, experimental insight into the underlying atomistic processes is still lacking due to the complexity of such measurements. Herein, atomic resolution electron tomography is performed on the same mesoporous-silica-coated gold nanorod, before and after femtosecond laser irradiation, to assess the missing information. Combined with molecular dynamics (MD) simulations based on the experimentally determined 3D atomic-scale morphology, the complex atomistic rearrangements, causing shape deformations and defect generation, are unraveled. These rearrangements are simultaneously driven by surface diffusion, facet restructuring, and strain formation, and are influenced by subtleties in the atomic distribution at the surface.

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3D Atomic-Scale Dynamics of Laser-Light-Induced Restructuring of Nanoparticles Unraveled by Electron Tomography

Abstract

Bibliographical note

Funding

Keywords

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