Electron- and light-induced stimulated Raman spectroscopy for nanoscale molecular mapping

Amr A. E. Saleh, Daniel K. Angell, and Jennifer A. Dionne
Phys. Rev. B 102, 085406 – Published 6 August 2020

Abstract

We propose and theoretically analyze a vibrational spectroscopy imaging technique, termed, termed electron- and light-induced stimulated Raman (ELISR) scattering, that combines the high spatial resolution of electron microscopy with the molecular sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but spatially-confined Stokes beam in the presence of a diffraction-limited pump laser. To characterize this technique, we develop a numerical model and conduct full-field electromagnetic simulations to investigate two distinct nanoparticle geometries, nanorods, and nanospheres, coated with a Raman-active material. Our results show the significant (106107) stimulated Raman enhancement that is achieved with dual electron and optical excitation of these nanoparticle geometries. Importantly, the spatial resolution of this vibrational spectroscopy for electron microscopy is solely determined by the nanoparticle geometry and the plasmon mode volume. Our results highlight the promise of ELISR for simultaneous high-resolution electron microscopy with sub-diffraction-limited Raman spectroscopy, complementing advances in super-resolution microscopy, correlated light and electron microscopy, and vibrational electron energy loss spectroscopy.

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  • Received 31 January 2020
  • Revised 9 July 2020
  • Accepted 10 July 2020

DOI:https://doi.org/10.1103/PhysRevB.102.085406

©2020 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Amr A. E. Saleh1,2,*,†, Daniel K. Angell1,*, and Jennifer A. Dionne1,3,‡

  • 1Materials Science and Engineering Dept., Stanford University, Stanford, California 94305, USA
  • 2Department of Engineering Mathematics and Physics, Faculty of Engineering, Cairo University, Giza 12613, Egypt
  • 3Department of Radiology, Molecular Imaging Program at Stanford (MIPS), Stanford University School of Medicine, Stanford, California 94305, USA

  • *These authors contributed equally to this work.
  • Corresponding author: aessawi@stanford.edu
  • Corresponding author: jdionne@stanford.edu

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Issue

Vol. 102, Iss. 8 — 15 August 2020

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