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Boltzmann-Distribution-Driven Cathodoluminescence Thermometry in In Situ Transmission Electron Microscopy
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    Boltzmann-Distribution-Driven Cathodoluminescence Thermometry in In Situ Transmission Electron Microscopy
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    • Pavel K. Olshin
      Pavel K. Olshin
      Department of Chemistry, College of Natural Sciences, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea
    • Won-Woo Park
      Won-Woo Park
      Department of Chemistry, College of Natural Sciences, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea
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    • Ye-Jin Kim
      Ye-Jin Kim
      Department of Chemistry, College of Natural Sciences, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea
      More by Ye-Jin Kim
    • Ye-Jin Choi
      Ye-Jin Choi
      Department of Chemistry, College of Natural Sciences, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea
      More by Ye-Jin Choi
    • Daria V. Mamonova
      Daria V. Mamonova
      Department of Chemistry, St. Petersburg State University, St. Petersburg 199034, Russia
    • Ilya E. Kolesnikov
      Ilya E. Kolesnikov
      Center for Optical and Laser Materials Research, St. Petersburg State University, St. Petersburg 199034, Russia
    • Elena V. Afanaseva
      Elena V. Afanaseva
      Department of Chemistry, Peter the Great St. Petersburg Polytechnic University, St. Petersburg 195251, Russia
    • Oh-Hoon Kwon*
      Oh-Hoon Kwon
      Department of Chemistry, College of Natural Sciences, Ulsan National Institute of Science and Technology, Ulsan 44919, Republic of Korea
      *Email: [email protected]
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    ACS Nano

    Cite this: ACS Nano 2024, 18, 49, 33441–33451
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    https://doi.org/10.1021/acsnano.4c10126
    Published November 27, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Nanothermometry in in situ transmission electron microscopy (TEM) is useful for comprehending the functioning mechanisms of the heterogeneous matter through real-time observations. Herein, we introduce a Boltzmann-distribution-driven cathodoluminescence (CL) nanothermometry for in situ local temperature probing in TEM. The population distribution across the close-lying Stark sublevels of dysprosium ions in an yttrium vanadate matrix follows the Boltzmann distribution, enabling the use of the CL-intensity ratio as a thermometry over a wide temperature range of 103–435 K with a relative sensitivity exceeding 3% K–1 and precision of ±2%. Superior to other CL-based thermometries, the present approach is independent of electron–beam parameters and dopant concentration, extending the robustness and applicability of CL-based nanothermometry in electron microscopy. We further demonstrate the real-time mapping of the temperature distribution across a TEM grid under laser irradiation.

    Copyright © 2024 American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c10126.

    • Deconvolution of the BG from the CL spectrum of YVO4:Dy3+, temperature-dependent CL of Dy3+ and YVO4, deconvolution of the emission peaks for the 4F9/26H11/2 transition, ratiometric CL thermometry based on Stark sublevels with various peaks, temperature-dependent CLIR with Stark sublevels at different concentrations of Dy3+, dependence of CLIR on the low electron-dose rate, dependence of CLIR on the high electron-dose rate, test for the relative precision of the temperature-calibration curves via intercept correction, averaged relative precision of the CL nanothermometry, size distribution of the particles, accuracy of the nanothermometry as a function of CL counts, in situ temperature measurements at a different mesh of the TEM grid, and electron-beam resistance of a single YVO4:Dy3+ particle (PDF)

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    ACS Nano

    Cite this: ACS Nano 2024, 18, 49, 33441–33451
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c10126
    Published November 27, 2024
    Copyright © 2024 American Chemical Society

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