Photoemission spectroscopy and microscopy for Ta@Si16 superatoms and their assembled layers

Abstract

Superatoms (SAs) with specific compositions have the potential to significantly advance the field of nanomaterials science, leading to next-generation nanoscale functionalities. In this study, we fabricated assembled layers with tantalum metal-atom encapsulating silicon cage (Ta@Si16) SAs on an organic C60 substrate through deposition, and we characterized their electronic and optical properties by photoelectron spectroscopy and microscopy. The alkaline nature of Ta@Si16 SAs reveals their electronic behaviors, such as charge transfer and electromagnetic near-field sensing, through two-photon photoemission (2PPE) spectroscopy and microscopy with a femtosecond laser. The evolution of the work function for Ta@Si16 SAs on C60, observed by 2PPE spectroscopy, demonstrates charge transfer complexation between the topmost C60 layer and the first Ta@Si16 layer, consistent with the electron-donating alkaline characteristics of Ta@Si16 SAs. Specifically, a small amount of Ta@Si16 SA deposition leads to a dramatic increase in 2PPE intensity, attributable to electromagnetic near-field enhancements, suggesting applications as sensitizers for nonlinear imaging in photoemission microscopy. For the assembled Ta@Si16 SA layers, a plasmonic response of p = 17.9 eV is spectroscopically identified, including their valence and conduction band structures, and the plasmonic energetics are discussed in the context of metal doping in bulk silicon.

Graphical abstract: Photoemission spectroscopy and microscopy for Ta@Si16 superatoms and their assembled layers

Supplementary files

Article information

Article type
Paper
Submitted
05 Jul 2024
Accepted
27 Oct 2024
First published
29 Oct 2024
This article is Open Access
Creative Commons BY-NC license

Nanoscale, 2024, Advance Article

Photoemission spectroscopy and microscopy for Ta@Si16 superatoms and their assembled layers

M. Shibuta, T. Ohta, T. Kamoshida, K. Yamagiwa, H. Tsunoyama, T. Inoue, T. Masubuchi and A. Nakajima, Nanoscale, 2024, Advance Article , DOI: 10.1039/D4NR02778G

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