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  1. Abstract

    Spatially resolved in situ transmission electron microscopy (TEM), equipped with direct electron detection systems, is a suitable technique to record information about the atom-scale dynamics with millisecond temporal resolution from materials. However, characterizing dynamics or fluxional behavior requires processing short time exposure images which usually have severely degraded signal-to-noise ratios. The poor signal-to-noise associated with high temporal resolution makes it challenging to determine the position and intensity of atomic columns in materials undergoing structural dynamics. To address this challenge, we propose a noise-robust, processing approach based on blob detection, which has been previously established for identifying objects in images in the community of computer vision. In particular, a blob detection algorithm has been tailored to deal with noisy TEM image series from nanoparticle systems. In the presence of high noise content, our blob detection approach is demonstrated to outperform the results of other algorithms, enabling the determination of atomic column position and its intensity with a higher degree of precision.

  2. Free, publicly-accessible full text available August 1, 2023
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  8. Abstract In this work, we employ density functional theory simulations to investigate possible spin polarization of CeO 2 -(111) surface and its impact on the interactions between a ceria support and Pt nanoparticles. With a Gaussian type orbital basis, our simulations suggest that the CeO 2 -(111) surface exhibits a robust surface spin polarization due to the internal charge transfer between atomic Ce and O layers. In turn, it can lower the surface oxygen vacancy formation energy and enhance the oxide reducibility. We show that the inclusion of spin polarization can significantly reduce the major activation barrier in the proposed reaction pathway of CO oxidation on ceria-supported Pt nanoparticles. For metal-support interactions, surface spin polarization enhances the bonding between Pt nanoparticles and ceria surface oxygen, while CO adsorption on Pt nanoparticles weakens the interfacial interaction regardless of spin polarization. However, the stable surface spin polarization can only be found in the simulations based on the Gaussian type orbital basis. Given the potential importance in the design of future high-performance catalysts, our present study suggests a pressing need to examine the surface ferromagnetism of transition metal oxides in both experiment and theory.
    Free, publicly-accessible full text available April 22, 2023
  9. null (Ed.)
    A deep convolutional neural network has been developed to denoise atomic-resolution transmission electron microscope image datasets of nanoparticles acquired using direct electron counting detectors, for applications where the image signal is severely limited by shot noise. The network was applied to a model system of CeO 2 -supported Pt nanoparticles. We leverage multislice image simulations to generate a large and flexible dataset for training the network. The proposed network outperforms state-of-the-art denoising methods on both simulated and experimental test data. Factors contributing to the performance are identified, including (a) the geometry of the images used during training and (b) the size of the network's receptive field. Through a gradient-based analysis, we investigate the mechanisms learned by the network to denoise experimental images. This shows that the network exploits both extended and local information in the noisy measurements, for example, by adapting its filtering approach when it encounters atomic-level defects at the nanoparticle surface. Extensive analysis has been done to characterize the network's ability to correctly predict the exact atomic structure at the nanoparticle surface. Finally, we develop an approach based on the log-likelihood ratio test that provides a quantitative measure of the agreement between the noisy observation and the atomic-levelmore »structure in the network-denoised image.« less