Light Emission Enhancement on Nanostructured Surfaces Nanoscopicaly Probed by Photon Correlation Cathodoluminescence

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Light Emission Enhancement on Nanostructured Surfaces Nanoscopicaly Probed by Photon Correlation Cathodoluminescence

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Author(s): Tomoyasu Fujimaru ¹ , Hiromu Tanaka ¹ , Masato Inamata ¹ , Midori Ikeuchi ² , Hidehiro Yamashita ² , Hiroya Miyazaki ³ , Takashi Gondo ³ , Satoshi Hata ¹ , Mitsuhiro Murayama ² ^, ⁴ , Hikaru Saito ² ^,

Publication date (Electronic): 21 January 2025

Conference name: 13th Asia Pacific Microscopy Congress 2025 (APMC13)

Conference date: 2-7 Febuary 2025

Keywords: light emission enhancement, halide perovskite, surface plasmon, cathodoluminescence, photon correlation

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Abstract

Nanostructures such as noble metal nanoparticles can enhance the light-matter interaction, and thus, nano-spectroscopy that can evaluate optical properties far beyond the diffraction limit of light is required. Cathodoluminescence (CL) spectroscopy has nanometer spatial resolution, however it is not straightforward to evaluate the light emission enhancement in integrated systems of materials and resonators because the electron beam excites not only materials but also resonators due to the lack of excitation wavelength selectivity. Recently, Hanbury Brown-Twiss (HBT) interferometry has been introduced into CL spectroscopy, which revealed that incoherent emission from classical emitters exhibits remarkable photon bunching [ 1]. It was also revealed that the measured second-order autocorrelation function g ⁽²⁾(τ) contains the excitation efficiency [ 2]. In this study, we apply HBT-CL to halide perovskite films on plasmonic resonator array, and successfully evaluate the emission enhancement. The experiment was carried out using a scanning transmission electron microscope (STEM) JEM-3200FSK (JEOL) under development for the "excitation event-selective CL microscope" at Kyushu University. The CL experiments were operated at an accelerating voltage of 300 kV. In this optical system ( Fig. 1(a)), a half mirror is used to split the photon path into two, and the photons are detected by a pair of single photon counting detectors (SPCDs). Another STEM Titan Cubed G2 (Thermo Fisher Scientific) was used for the compositional and chemical analyses of the samples. This microscope was operated at an accelerating voltage of 80 kV. The sample used is a light-emitting thin film deposited on a plasmonic resonator array. Specifically, a CsPbBr ₃/Cs ₄PbBr ₆ (CPB) nanocomposite, in which CsPbBr ₃ nanoparticles are dispersed in Cs ₄PbBr ₆, is used as the thin film, and Al disks with a diameter of 160 nm and a height of 30 nm are arranged in a square lattice with a period of 350 nm ( Fig. 2).

Fig. 1

Schematic of the STEM-CL setup. CL is collimated by a parabolic mirror and transferred to a spectrometer or an HBT interferometer.

Fig. 2

(a) Schematic of the cross section of the sample, (b) An annular dark-field (ADF)-STEM image, (c) Al, (d) Cs, (e) Pb maps obtained by EDS.

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Publication date (Electronic): 21 January 2025

Electronic Location Identifier: e267

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[1 ]Interdisciplinary Graduate School of Engineering Sciences, Kyushu University, Kasuga, Fukuoka, Japan

[2 ]Institute for Materials Chemistry and Engineering, Kyushu University, Kasuga, Fukuoka, Japan

[3 ]Mel-Build Corporation, Nishi-ku, Fukuoka, Japan

[4 ]Department of Materials Science and Engineering, Virginia Tech, Blacksburg, Virginia, United States

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*Corresponding author: saito.hikaru.961@ 123456m.kyushu-u.ac.jp

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Tomoyasu Fujimaru https://orcid.org/0009-0000-8808-068X

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DOI: 10.14293/APMC13-2025-0267

SO-VID: 7385b30c-4163-42cc-b82f-a64224100a6c

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Published under Creative Commons Attribution 4.0 International ( CC BY 4.0). Users are allowed to share (copy and redistribute the material in any medium or format) and adapt (remix, transform, and build upon the material for any purpose, even commercially), as long as the authors and the publisher are explicitly identified and properly acknowledged as the original source.

Conference name: 13th Asia Pacific Microscopy Congress 2025

Conference acronym: APMC13

Conference number: 13

Conference location: Brisbane, Australia

Conference date: 2-7 Febuary 2025

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References

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[1] S. Meuret, L. H. G. Tizei, T. Cazimajou, R. Bourrellier, H. C. Chang, F. Treussart, and M. Kociak, Phys. Rev. Lett. 114, 197401 (2015). https://doi.org/10.1103/PhysRevLett.114.197401

[2] S. Yanagimoto, N. Yamamoto, T. Sannomiya, and K. Akiba, Phys. Rev. B 103, 205418 (2021). https://doi.org/10.1103/PhysRevB.103.205418

[3] T. Kubota, S. Yanagimoto, H. Saito, K. Akiba, A. Ishii, and T. Sannomiya, Appl. Phys. Express 17, 015005 (2024). https://doi.org/10.35848/1882-0786/ad1bc4

[4] Y. Li, L. Chen, B. Liu, J. Ruan, J. Liu, X. Ouyang, and Q. Xu, Ceram. Int. 48, 16730–16736 (2022). https://doi.org/10.1016/j.ceramint.2022.02.222

Light Emission Enhancement on Nanostructured Surfaces Nanoscopicaly Probed by Photon Correlation Cathodoluminescence

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