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

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.

doi:10.1063/1.5096595

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

Journal Article · 05 August 2019 · Applied Physics Letters

DOI: https://doi.org/10.1063/1.5096595 · OSTI ID:1568817

^[1]; Stevens, A. ^[2]; Kovarik, L. ^[3]; Jiang, N. ^[4]; Mehta, H. ^[3]; Liyu, A. ^[3]; Reehl, S. ^[3];

^[3]; Luzi, L. ^[3]; Hao, W. ^[3]; Bramer, L. ^[3]; Browning, N. D. ^[5]

Univ. of Liverpool (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sivananthan Lab., Bolingbrook, IL (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Arizona State Univ., Tempe, AZ (United States)
Univ. of Liverpool (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Sivananthan Lab., Bolingbrook, IL (United States)

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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1568817

Alternate ID(s):: OSTI ID: 1546867

Report Number(s):: PNNL-SA-145156; TRN: US2001106

Journal Information:: Applied Physics Letters, Vol. 115, Issue 6; ISSN 0003-6951

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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