3D imaging of Circular Dichroic Plasmonic Near-Fields Using Polarization-Controlled Photo-Induced Near-Field Electron Microscopy (PINEM)

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3D imaging of Circular Dichroic Plasmonic Near-Fields Using Polarization-Controlled Photo-Induced Near-Field Electron Microscopy (PINEM)

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Author(s): Jaeyeon Jo ¹ , Haihua Liu ² , In Han Ha ¹ , Ingyu Yoo ¹ , Jian-min Zuo ³ ^, , Ki Tae Nam ¹ ^, , Miyoung Kim ¹ ^,

Publication date (Electronic): 21 January 2025

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

Conference date: 2-7 Febuary 2025

Keywords: Plasmonics, Chiral Au nanoparticle, PINEM, EELS, tomography

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Abstract

Plasmonic near-fields in chiral nanoparticles exhibiting circular dichroism—differential absorption based on the handedness of circularly polarized light—vary with the polarization of the incident light. These polarization-dependent near-fields hold potential as platforms for locally enhanced chiral light-matter interactions, with promising applications in enantioselective biosensing and photocatalysis [ 1]. To fully understand and utilize these chiral near-fields, it is essential to identify where the fields are strongest within the nanoparticles. Electron spectroscopy in a Transmission Electron Microscope is a suitable technique for mapping plasmonic fields, offering high spatial resolution and the simultaneous collection of imaging and spectroscopic data. The spectroscopy can even possess sensitivity to polarization-dependence when coupled with laser in an ultrafast electron microscope (UEM). In UEM, left-d or right-handed circularly polarized laser light selectively excites the chiral near-fields, while the electron beam probes them with nanometer resolution [ 2- 3]. One technique, called photon-induced near-field electron microscopy (PINEM) developed in UEM, enables nanoscale mapping of the chiral response of near-fields.

Here, we employed PINEM in conjunction with a tomographic approach to observe the plasmonic fields of a chiral gold nanoparticle in 3D. Helicoid III nanoparticles were selected as a model system for their large dissymmetry factor, presenting a complex 3D shape ( Figure 1a) that necessitates volumetric analysis of their near-fields [ 4]. By tilting the specimen from -48° to +50° relative to the fixed laser and electron beam direction, 10 sets of PINEM images were acquired under left- and right-handed circularly polarized light with a wavelength of 650 nm. By aligning the centers of the PINEM images at each tilt angle—using manual corner detections followed by several stages of image refinement—a tilt series of circular dichroic plasmonic maps was obtained ( Figure 1b).

Fig. 1

a) Circular dichroism (differential absorbance between left- and right-handed circularly polarized light) and calculated optical helicity, a value proportional to circular dichroism, for Helicoid III nanoparticles. The 3D shape of the nanoparticle obtained through electron tomography is shown in the inset. b) Images from a tilt series of circular dichroic PINEM projections, where positive values indicate a stronger signal for left-handed circular polarization. Intensities were normalized for each image, and the tilt angle of the specimen is shown below each image. Pixel size = 2.3 nm x 2.3 nm.

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Publication date (Electronic): 21 January 2025

Electronic Location Identifier: e278

Affiliations

[1 ]Department of Materials Science and Engineering, Seoul National University, Seoul, Republic of Korea

[2 ]Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, United States

[3 ]Department of Materials Science and Engineering, University of Illinois – Urbana-Champaign, Urbana, IL, United States

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*Corresponding authors: jianzuo@ 123456illinois.edu , nkitae@ 123456snu.ac.kr , mkim@ 123456snu.ac.kr

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Jaeyeon Jo https://orcid.org/0000-0003-0982-042X

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DOI: 10.14293/APMC13-2025-0278

SO-VID: ab348eb1-3970-404a-993f-01f65c63e3c4

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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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Funding

Funded by: National Research Foundation of Korea (NRF)

Award ID: NRF-2022R1A2C3007807

Funded by: U.S. DOE, Office of Basic Energy Sciences

Award ID: DE-AC02-06CH11357

M. Kim acknowledges the financial support from National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2022R1A2C3007807). The ultrafast electron microscopy was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

References

R. M. Kim, et al., Nature 612 (2022), p. 470. https://doi.org/10.1038/s41586-022-05383-9
S. Zhou, et al., Nature 612 (2022), p. 259. https://doi.org/10.1038/s41586-022-05340-6
H. Liu, et al., Nano Letters 21 (2021), p. 5842. https://doi.org/10.1021/acs.nanolett.1c01361
H.-E. Lee, et al., Nature 556 (2018), p. 360. https://doi.org/10.1038/s41586-018-0034-1
R. Leary et al., Ultramicroscopy 131 (2013), p. 70. https://doi.org/10.1016/j.ultramic.2013.03.019

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[1] R. M. Kim, et al., Nature 612 (2022), p. 470. https://doi.org/10.1038/s41586-022-05383-9

[2] S. Zhou, et al., Nature 612 (2022), p. 259. https://doi.org/10.1038/s41586-022-05340-6

[3] H. Liu, et al., Nano Letters 21 (2021), p. 5842. https://doi.org/10.1021/acs.nanolett.1c01361

[4] H.-E. Lee, et al., Nature 556 (2018), p. 360. https://doi.org/10.1038/s41586-018-0034-1

[5] R. Leary et al., Ultramicroscopy 131 (2013), p. 70. https://doi.org/10.1016/j.ultramic.2013.03.019

3D imaging of Circular Dichroic Plasmonic Near-Fields Using Polarization-Controlled Photo-Induced Near-Field Electron Microscopy (PINEM)

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