Research ArticleCHEMICAL PHYSICS

Real-space analysis of diffusion behavior and activation energy of individual monatomic ions in a liquid

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Science Advances  15 Dec 2017:
Vol. 3, no. 12, e1701546
DOI: 10.1126/sciadv.1701546
  • Fig. 1 Schematic representation of the observation method.

    Monatomic ion–dispersed ionic liquid forms ultrathin films in holes of a thin carbon film, and the electron beam is focused on the liquid film.

  • Fig. 2 Atomic-resolution imaging of monatomic gold ions in C2mimTFSI.

    (A and B) Simultaneously obtained bright-field and ADF images. The inset at the bottom-right corner in (B) is the simulated image of a gold ion in C2mimTFSI. (C) Left: Enlarged image of spot A and the simulated image in (B). (D) Intensity profiles of spot A and the simulated image in (C). arb. units, arbitrary units. (E) Histogram of the spot areas in (B).

  • Fig. 3 Atomic diffusion analysis.

    (A) Continuous ADF images taken at a rate of 4.2 s per frame. The selected ions are labeled as A, B, and C. (B) Trajectory of the ions in (A). The labels A, B, and C are the same as those in (A). (C) Trajectory of spot C in (B). Each circled point is the position of ion C at the corresponding time. (D) Histogram of the atomic displacement within the duration of one frame. The left and right axes correspond to the number of ions and the integrated rate of the total number, respectively. (E) Mean square displacement (MSD) of the ions as a function of time.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/3/12/e1701546/DC1

    section S1. ADF observation of different compositions (C8mimCl-Au, C2mimTFSI-I, and C8mimCl-I)

    section S2. Multislice image simulation for thickness, defocus, and composition dependence

    section S3. Splitting spot analysis

    section S4. Confirmation of the isotropic displacement

    section S5. Diffusion coefficient of gold ions in the liquid phase

    section S6. Electron-beam effects

    fig. S1. Shape change of the liquid films by tilting the sample.

    fig. S2. Direct imaging of gold and iodine ions in liquids.

    fig. S3. Schematic structures for the ADF simulations.

    fig. S4. Dependence of the ADF images of the gold atoms on the thickness of the liquid phase.

    fig. S5. Dependence of the ADF images of the gold and iodine atoms on the defocus.

    fig. S6. Dependence of the ADF images on the liquid composition.

    fig. S7. Imaging time of each bright spot.

    fig. S8. Splitting spot analysis.

    fig. S9. Confirmation of the isotropic displacement of the gold ions.

    fig. S10. Electron beam effect: Steady heat conduction.

    fig. S11. Electron beam effect: Nonsteady heat conduction.

    fig. S12. Relationships between the parameters involved in elastic scattering.

    fig. S13. Dose rate density dependence of diffusion coefficient of gold ions in a film.

    table S1. Displacement cross sections for atomic species with different displacement energies (Ed) at an accelerating voltage of 200 kV.

    movie S1. Motion of gold monatomic ions in C2mimTFSI.

    References (2238)

  • Supplementary Materials

    This PDF file includes:

    • section S1. ADF observation of different compositions (C8mimCl-Au, C2mimTFSI-I, and C8mimCl-I)
    • section S2. Multislice image simulation for thickness, defocus, and composition dependence
    • section S3. Splitting spot analysis
    • section S4. Confirmation of the isotropic displacement
    • section S5. Diffusion coefficient of gold ions in the liquid phase
    • section S6. Electron-beam effects
    • fig. S1. Shape change of the liquid films by tilting the sample.
    • fig. S2. Direct imaging of gold and iodine ions in liquids.
    • fig. S3. Schematic structures for the ADF simulations.
    • fig. S4. Dependence of the ADF images of the gold atoms on the thickness of the liquid phase.
    • fig. S5. Dependence of the ADF images of the gold and iodine atoms on the defocus.
    • fig. S6. Dependence of the ADF images on the liquid composition.
    • fig. S7. Imaging time of each bright spot.
    • fig. S8. Splitting spot analysis.
    • fig. S9. Confirmation of the isotropic displacement of the gold ions.
    • fig. S10. Electron beam effect: Steady heat conduction.
    • fig. S11. Electron beam effect: Nonsteady heat conduction.
    • fig. S12. Relationships between the parameters involved in elastic scattering.
    • fig. S13. Dose rate density dependence of diffusion coefficient of gold ions in a film.
    • table S1. Displacement cross sections for atomic species with different displacement energies (Ed) at an accelerating voltage of 200 kV.
    • References (22–38)

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    Other Supplementary Material for this manuscript includes the following:

    • movie S1 (.avi format). Motion of gold monatomic ions in C2mimTFSI.

    Files in this Data Supplement:

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