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ACS Publications. Most Trusted. Most Cited. Most Read
Imaging Nanometer Phonon Softening at Crystal Surface Steps with 4D Ultrafast Electron Microscopy

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Nano Lett. 2021, 21, 17, 7332-7338
    Letter

    Imaging Nanometer Phonon Softening at Crystal Surface Steps with 4D Ultrafast Electron Microscopy
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    • Yichao Zhang
      Yichao Zhang
      Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, Minnesota 55455, United States
      More by Yichao Zhang
    • David J. Flannigan*
      David J. Flannigan
      Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, Minnesota 55455, United States
      *E-mail: [email protected]
      More by David J. Flannigan
      Orcidhttps://orcid.org/0000-0002-1829-1868
    Other Access OptionsSupporting Information (2)

    Nano Letters

    Cite this: Nano Lett. 2021, 21, 17, 7332–7338
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    https://doi.org/10.1021/acs.nanolett.1c02524
    Published August 18, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Step edges are an important and prevalent topological feature that influence catalytic, electronic, vibrational, and structural properties arising from modulation of atomic-scale force fields due to edge-atom relaxation. Direct probing of ultrafast atomic-to-nanoscale lattice dynamics at individual steps poses a particularly significant challenge owing to demanding spatiotemporal resolution requirements. Here, we achieve such resolutions with femtosecond 4D ultrafast electron microscopy and directly image nanometer-variant softening of photoexcited phonons at individual surface steps. We find large degrees of softening precisely at the step position, with a thickness-dependent, strain-induced frequency modulation extending tens of nanometers laterally from the atomic-scale discontinuity. The effect originates from anisotropic bond dilation and photoinduced incoherent atomic displacements delineated by abrupt molecular-layer cessation. The magnitude and spatiotemporal extent of softening is quantitatively described with a finite-element transient-deformation model. The high spatiotemporal resolutions demonstrated here enable uncovering of new insights into atomic-scale structure–function relationships of highly defect-sensitive, functional materials.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.1c02524.

    • Additional Materials and Methods describing preliminary TEM structural characterization, nanometer spatial mapping of the onset of fs photoinduced phonon dynamics, details of the nanometer spatial mapping of phonon softening at the step, details of the method for determining crystal thickness in each ROI, calculation of the photoinduced c-axis strain profile in the layer-stacking direction of each ROI, and details of the finite-element transient-deformation analysis (PDF)

    • Video 1: High spatiotemporal-resolution UEM video of phonon dynamics at a step edge in an ultrathin 2H-MoS2 flake (AVI)

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    Cited By

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    This article is cited by 8 publications.

    1. Margaret L. Clapham, Aritra Das, Christopher J. Douglas, Renee R. Frontiera. Killer Phonon Caught: Femtosecond Stimulated Raman Spectroscopy Identifies Phonon-Induced Control of Photophysics in Rubrene Derivatives. Journal of the American Chemical Society 2024, 146 (29) , 19939-19950. https://doi.org/10.1021/jacs.4c03249
    2. Kuai Yu, Guo Ping Wang. Coherent Acoustic Vibrational Spectrum of Single and Coupled Nanoresonators. The Journal of Physical Chemistry C 2024, 128 (13) , 5394-5407. https://doi.org/10.1021/acs.jpcc.4c00256
    3. Parivash Moradifar, Yin Liu, Jiaojian Shi, Matti Lawton Siukola Thurston, Hendrik Utzat, Tim B. van Driel, Aaron M. Lindenberg, Jennifer A. Dionne. Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy. Chemical Reviews 2023, 123 (23) , 12757-12794. https://doi.org/10.1021/acs.chemrev.2c00917
    4. Faran Zhou, Haihua Liu, Marc Zajac, Kyle Hwangbo, Qianni Jiang, Jiun-Haw Chu, Xiaodong Xu, Ilke Arslan, Thomas E. Gage, Haidan Wen. Ultrafast Nanoimaging of Spin-Mediated Shear Waves in an Acoustic Cavity. Nano Letters 2023, 23 (22) , 10213-10220. https://doi.org/10.1021/acs.nanolett.3c02747
    5. Francis M. Alcorn, Maya Chattoraj, Renske M. van der Veen, Prashant K. Jain. Watching Plasmon-Induced Nanoparticle Ostwald Ripening. The Journal of Physical Chemistry C 2023, 127 (33) , 16538-16544. https://doi.org/10.1021/acs.jpcc.3c04035
    6. Francis M. Alcorn, Prashant K. Jain, Renske M. van der Veen. Time-resolved transmission electron microscopy for nanoscale chemical dynamics. Nature Reviews Chemistry 2023, 16 https://doi.org/10.1038/s41570-023-00469-y
    7. N. Bach, A. Feist, M. Möller, C. Ropers, S. Schäfer. Tailored nanophononic wavefield in a patterned bilayer system probed by ultrafast convergent beam electron diffraction. Structural Dynamics 2022, 9 (3) , 034301. https://doi.org/10.1063/4.0000144
    8. Ryan A. Gnabasik, Pranav K. Suri, Jialiang Chen, David J. Flannigan. Imaging coherent phonons and precursor dynamics in LaFeAsO with 4D ultrafast electron microscopy. Physical Review Materials 2022, 6 (2) https://doi.org/10.1103/PhysRevMaterials.6.024802
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    Nano Letters

    Cite this: Nano Lett. 2021, 21, 17, 7332–7338
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.1c02524
    Published August 18, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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