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Title: Controlling the spatio-temporal dose distribution during STEM imaging by subsampled acquisition: In-situ observations of kinetic processes in liquids

Abstract

Subsampled image acquisition followed by image inpainting in the scanning transmission electron microscope (STEM) is a novel approach to control dose and increase the image frame rate during experiments, thereby allowing independent control of the spatial and temporal dose envelope during image acquisition. Here, subsampled imaging is shown to permit precise in-situ observations of the fundamental kinetic processes behind nucleation and growth of silver (Ag) nanoparticles from an aqueous solution. At high sampling-levels, nanoparticles can be observed with morphologies that are consistent with strong interface interactions, i.e. rafts and pillars, whereas at low sampling-levels, the particles exhibit regular spherical morphologies. The relative numbers of rafts/pillars and regular nanoparticles, their sizes and their incubation times can be attributed to local changes in the molar concentration of the Ag ions in the aqueous solution; higher sampling-levels significantly increase the reactants in the vicinity of the window, leading to rapid supersaturation and the precipitation on the window surface. These precisely controlled kinetics highlight subsampled imaging as a method by which the driving force for nucleation and growth (i.e the electron beam) can be disentangled from the spatial/temporal resolution of the observation in all in-situ experiments, providing a pathway to identify and quantify themore » importance of individual kinetic factors behind nucleation and growth in a wide variety of complex materialssystems and architectures.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3];  [3];  [3]; ORCiD logo [3];  [3];  [3];  [3];  [5]
+ Show Author Affiliations
  1. Univ. of Liverpool (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Sivananthan Lab., Bolingbrook, IL (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Arizona State Univ., Tempe, AZ (United States)
  5. Univ. of Liverpool (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Sivananthan Lab., Bolingbrook, IL (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1568817
Alternate Identifier(s):
OSTI ID: 1546867
Report Number(s):
PNNL-SA-145156
Journal ID: ISSN 0003-6951; TRN: US2001106
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 115; Journal Issue: 6; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Mehdi, B. L., Stevens, A., Kovarik, L., Jiang, N., Mehta, H., Liyu, A., Reehl, S., Stanfill, B., Luzi, L., Hao, W., Bramer, L., and Browning, N. D.. Controlling the spatio-temporal dose distribution during STEM imaging by subsampled acquisition: In-situ observations of kinetic processes in liquids. United States: N. p., 2019. Web. doi:10.1063/1.5096595.
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Mehdi, B. L., Stevens, A., Kovarik, L., Jiang, N., Mehta, H., Liyu, A., Reehl, S., Stanfill, B., Luzi, L., Hao, W., Bramer, L., & Browning, N. D.. Controlling the spatio-temporal dose distribution during STEM imaging by subsampled acquisition: In-situ observations of kinetic processes in liquids. United States. https://doi.org/10.1063/1.5096595
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Mehdi, B. L., Stevens, A., Kovarik, L., Jiang, N., Mehta, H., Liyu, A., Reehl, S., Stanfill, B., Luzi, L., Hao, W., Bramer, L., and Browning, N. D.. Mon . "Controlling the spatio-temporal dose distribution during STEM imaging by subsampled acquisition: In-situ observations of kinetic processes in liquids". United States. https://doi.org/10.1063/1.5096595. https://www.osti.gov/servlets/purl/1568817.
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@article{osti_1568817,
title = {Controlling the spatio-temporal dose distribution during STEM imaging by subsampled acquisition: In-situ observations of kinetic processes in liquids},
author = {Mehdi, B. L. and Stevens, A. and Kovarik, L. and Jiang, N. and Mehta, H. and Liyu, A. and Reehl, S. and Stanfill, B. and Luzi, L. and Hao, W. and Bramer, L. and Browning, N. D.},
abstractNote = {Subsampled image acquisition followed by image inpainting in the scanning transmission electron microscope (STEM) is a novel approach to control dose and increase the image frame rate during experiments, thereby allowing independent control of the spatial and temporal dose envelope during image acquisition. Here, subsampled imaging is shown to permit precise in-situ observations of the fundamental kinetic processes behind nucleation and growth of silver (Ag) nanoparticles from an aqueous solution. At high sampling-levels, nanoparticles can be observed with morphologies that are consistent with strong interface interactions, i.e. rafts and pillars, whereas at low sampling-levels, the particles exhibit regular spherical morphologies. The relative numbers of rafts/pillars and regular nanoparticles, their sizes and their incubation times can be attributed to local changes in the molar concentration of the Ag ions in the aqueous solution; higher sampling-levels significantly increase the reactants in the vicinity of the window, leading to rapid supersaturation and the precipitation on the window surface. These precisely controlled kinetics highlight subsampled imaging as a method by which the driving force for nucleation and growth (i.e the electron beam) can be disentangled from the spatial/temporal resolution of the observation in all in-situ experiments, providing a pathway to identify and quantify the importance of individual kinetic factors behind nucleation and growth in a wide variety of complex materialssystems and architectures.},
doi = {10.1063/1.5096595},
journal = {Applied Physics Letters},
number = 6,
volume = 115,
place = {United States},
year = {2019},
month = {8}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5096595
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Cited by: 19 works
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Figures / Tables:

FIG. 1 FIG. 1: A set of subsampled images taken from different cumulative doses (i.e., time stamps) in the in situ nucleation and growth of Ag nanoparticles. For each of the images, the cumulative dose is controlled by the magnification, scan speed, and subsampling of the images. The videos from which thesemore » images were taken are shown in the supplementary material (SM1).« less
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