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Title: Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast

Abstract

Abstract The use of transmission electron microscopy (TEM) to observe real-time structural and compositional changes has proven to be a valuable tool for understanding the dynamic behavior of nanomaterials. However, identifying the nanoparticles of interest typically require an obvious change in position, size, or structure, as compositional changes may not be noticeable during the experiment. Oxidation or reduction can often result in subtle volume changes only, so elucidating mechanisms in real-time requires atomic-scale resolution or in-situ electron energy loss spectroscopy, which may not be widely accessible. Here, by monitoring the evolution of diffraction contrast, we can observe both structural and compositional changes in iron oxide nanoparticles, specifically the oxidation from a wüstite-magnetite (FeO@Fe 3 O 4 ) core – shell nanoparticle to single crystalline magnetite, Fe 3 O 4 nanoparticle. The in-situ TEM images reveal a distinctive light and dark contrast known as the ‘Ashby-Brown contrast’, which is a result of coherent strain across the core – shell interface. As the nanoparticles fully oxidize to Fe 3 O 4 , the diffraction contrast evolves and then disappears completely, which is then confirmed by modeling and simulation of TEM images. This represents a new, simplified approach to tracking the oxidation ormore » reduction mechanisms of nanoparticles using in-situ TEM experiments.« less

Authors:
; ; ; ; ORCiD logo; ; ORCiD logo
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
OSTI Identifier:
2203008
Alternate Identifier(s):
OSTI ID: 2009022; OSTI ID: 2203415
Report Number(s):
LA-UR-23-26777
Journal ID: ISSN 2515-7639
Grant/Contract Number:  
20210604ECR; 89233218CNA000001; NA0003525
Resource Type:
Published Article
Journal Name:
JPhys Materials
Additional Journal Information:
Journal Name: JPhys Materials Journal Volume: 6 Journal Issue: 4; Journal ID: ISSN 2515-7639
Publisher:
IOP Publishing
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE; in-situ; environmental TEM; oxidation; iron oxide nanoparticles; Ashby-Brown contrast

Citation Formats

Poerwoprajitno, Agus R., Baradwaj, Nitish, Singh, Manish Kumar, Carter, C. Barry, Huber, Dale L., Kalia, Rajiv, and Watt, John. Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast. United Kingdom: N. p., 2023. Web. doi:10.1088/2515-7639/ad025f.
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Poerwoprajitno, Agus R., Baradwaj, Nitish, Singh, Manish Kumar, Carter, C. Barry, Huber, Dale L., Kalia, Rajiv, & Watt, John. Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast. United Kingdom. https://doi.org/10.1088/2515-7639/ad025f
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Poerwoprajitno, Agus R., Baradwaj, Nitish, Singh, Manish Kumar, Carter, C. Barry, Huber, Dale L., Kalia, Rajiv, and Watt, John. Thu . "Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast". United Kingdom. https://doi.org/10.1088/2515-7639/ad025f.
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@article{osti_2203008,
title = {Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast},
author = {Poerwoprajitno, Agus R. and Baradwaj, Nitish and Singh, Manish Kumar and Carter, C. Barry and Huber, Dale L. and Kalia, Rajiv and Watt, John},
abstractNote = {Abstract The use of transmission electron microscopy (TEM) to observe real-time structural and compositional changes has proven to be a valuable tool for understanding the dynamic behavior of nanomaterials. However, identifying the nanoparticles of interest typically require an obvious change in position, size, or structure, as compositional changes may not be noticeable during the experiment. Oxidation or reduction can often result in subtle volume changes only, so elucidating mechanisms in real-time requires atomic-scale resolution or in-situ electron energy loss spectroscopy, which may not be widely accessible. Here, by monitoring the evolution of diffraction contrast, we can observe both structural and compositional changes in iron oxide nanoparticles, specifically the oxidation from a wüstite-magnetite (FeO@Fe 3 O 4 ) core – shell nanoparticle to single crystalline magnetite, Fe 3 O 4 nanoparticle. The in-situ TEM images reveal a distinctive light and dark contrast known as the ‘Ashby-Brown contrast’, which is a result of coherent strain across the core – shell interface. As the nanoparticles fully oxidize to Fe 3 O 4 , the diffraction contrast evolves and then disappears completely, which is then confirmed by modeling and simulation of TEM images. This represents a new, simplified approach to tracking the oxidation or reduction mechanisms of nanoparticles using in-situ TEM experiments.},
doi = {10.1088/2515-7639/ad025f},
journal = {JPhys Materials},
number = 4,
volume = 6,
place = {United Kingdom},
year = {Thu Oct 19 00:00:00 EDT 2023},
month = {Thu Oct 19 00:00:00 EDT 2023}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1088/2515-7639/ad025f
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