Radiolysis‐Driven Evolution of Gold Nanostructures – Model Verification by Scale Bridging In Situ Liquid‐Phase Transmission Electron Microscopy and X‐Ray Diffraction

Fritsch B, Zech T, Bruns M, Körner A, Khadivianazar S, Wu M, Zargar Talebi N, Virtanen S, Unruh T, Jank M, Spiecker E, Hutzler A (2022)

Publication Type: Journal article

Publication year: 2022

Journal

Advanced Science Wiley Open Access

Book Volume: 9

Article Number: 2202803

Journal Issue: 25

URI: https://onlinelibrary.wiley.com/doi/10.1002/advs.202202803

DOI: 10.1002/advs.202202803

Open Access Link: https://onlinelibrary.wiley.com/doi/10.1002/advs.202202803

Abstract

Utilizing ionizing radiation for in situ studies in liquid media enables unique insights into nanostructure formation dynamics. As radiolysis interferes with observations, kinetic simulations are employed to understand and exploit beam-liquid interactions. By introducing an intuitive tool to simulate arbitrary kinetic models for radiation chemistry, it is demonstrated that these models provide a holistic understanding of reaction mechanisms. This is shown for irradiated HAuCl4 solutions allowing for quantitative prediction and tailoring of redox processes in liquid-phase transmission electron microscopy (LP-TEM). Moreover, it is demonstrated that kinetic modeling of radiation chemistry is applicable to investigations utilizing X-rays such as X-ray diffraction (XRD). This emphasizes that beam-sample interactions must be considered during XRD in liquid media and shows that reaction kinetics do not provide a threshold dose rate for gold nucleation relevant to LP-TEM and XRD. Furthermore, it is unveiled that oxidative etching of gold nanoparticles depends on both, precursor concentration, and dose rate. This dependency is exploited to probe the electron beam-induced shift in Gibbs free energy landscape by analyzing critical radii of gold nanoparticles.

Authors with CRIS profile

Birk Fritsch Lehrstuhl für Werkstoffwissenschaften (Mikro- und Nanostrukturforschung) Tobias Zech Lehrstuhl für Kristallographie und Strukturphysik Mark Bruns Professur für Werkstoffwissenschaften (Korrosion und Oberflächentechnik) Andreas Körner Lehrstuhl für Elektrokatalyse (HIERN) Saba Khadivianazar Lehrstuhl für Elektronische Bauelemente Mingjian Wu Lehrstuhl für Werkstoffwissenschaften (Mikro- und Nanostrukturforschung) Neda Zargar Talebi Lehrstuhl für Elektronische Bauelemente Sannakaisa Virtanen Professur für Werkstoffwissenschaften (Korrosion und Oberflächentechnik) Tobias Unruh Professur für Nanomaterialcharakterisierung (Streumethoden) Michael Jank Lehrstuhl für Elektronische Bauelemente Erdmann Spiecker Lehrstuhl für Werkstoffwissenschaften (Mikro- und Nanostrukturforschung) Andreas Hutzler Lehrstuhl für Elektronische Bauelemente

Additional Organisation(s)

Graduiertenkolleg 1896/2 In situ Mikroskopie mit Elektronen, Röntgenstrahlen und Rastersonden Interdisziplinäres Zentrum, Center for Nanoanalysis and Electron Microscopy (CENEM)

How to cite

APA:

Fritsch, B., Zech, T., Bruns, M., Körner, A., Khadivianazar, S., Wu, M.,... Hutzler, A. (2022). Radiolysis‐Driven Evolution of Gold Nanostructures – Model Verification by Scale Bridging In Situ Liquid‐Phase Transmission Electron Microscopy and X‐Ray Diffraction. Advanced Science, 9(25). https://doi.org/10.1002/advs.202202803

MLA:

Fritsch, Birk, et al. "Radiolysis‐Driven Evolution of Gold Nanostructures – Model Verification by Scale Bridging In Situ Liquid‐Phase Transmission Electron Microscopy and X‐Ray Diffraction." Advanced Science 9.25 (2022).

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