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Updated: Feb 15, 2026

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Selective Coherent Anti-Stokes Raman Scattering Microscopy Employing Dual-Wavelength Nanofocused Ultrafast Plasmon

Keita Tomita1, Yasuhiro Kojima1, Fumihiko Kannari1

  • 1Department of Electronics and Electrical Engineering, Keio University , 3-14-1, Hiyoshi, Kohoku-ku, Yokohama, Kanagawa 223-8522, Japan.

Nano Letters
|January 30, 2018
PubMed
Summary

Ultrafast surface plasmon polariton nanofocusing enables background-free excitation. This dual-wavelength method enhances coherent anti-Stokes Raman scattering microscopy for nanoscale imaging of materials like graphene and carbon nanotubes.

Keywords:
Surface plasmon polaritonscoherent anti-Stokes Raman scatteringnanofocusingnonlinear microscopypulse shaping

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Area of Science:

  • Plasmonics
  • Nanophotonics
  • Spectroscopy

Background:

  • Ultrafast surface plasmon polariton (SPP) nanofocusing allows for localized excitation beyond the diffraction limit.
  • Plasmonic tapered tips are crucial for concentrating light at the nanoscale.

Purpose of the Study:

  • To demonstrate simultaneous nanofocusing of ultrafast SPP pulses at 440 and 800 nm.
  • To develop a selective coherent anti-Stokes Raman scattering (CARS) microscopy technique using dual-wavelength nanofocusing.

Main Methods:

  • Fabrication of an aluminum (Al) tapered tip with a common diffraction grating structure.
  • Coupling of femtosecond laser pulses at 440 nm (2ω) and 800 nm (ω) to the tapered tip for SPP generation.
  • Utilizing spectral focusing for selective vibrational excitation in CARS microscopy.

Main Results:

  • Achieved simultaneous nanofocusing of 440 nm and 800 nm SPP pulses to a tip apex radius of ~35 nm.
  • Demonstrated a novel 2ω-CARS microscopy technique with significantly enhanced Raman intensity (3.96x for G-band, 4.00x for 2D-band) for monolayer graphene compared to ω-CARS.
  • Successfully applied the 2ω-CARS imaging method for multiwalled carbon nanotubes, resolving D-, G-, and 2D-bands.

Conclusions:

  • Dual-wavelength SPP nanofocusing provides a powerful tool for nanoscale optical excitation and microspectroscopy.
  • The developed 2ω-CARS microscopy offers enhanced sensitivity and selectivity for material characterization.
  • This technique opens avenues for advanced nanoscale imaging and optical phenomena like sum frequency mixing and two-photon excitation.