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Visualizing hot carrier dynamics by nonlinear optical spectroscopy at the atomic length scale

Author

Listed:
  • Yang Luo

    (Max Planck Institute for Solid State Research)

  • Shaoxiang Sheng

    (Max Planck Institute for Solid State Research)

  • Andrea Schirato

    (Politecnico di Milano
    Rice University)

  • Alberto Martin-Jimenez

    (Max Planck Institute for Solid State Research
    Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanociencia))

  • Giuseppe Valle

    (Politecnico di Milano
    Istituto di Fotonica e Nanotecnologie – Consiglio Nazionale delle Ricerche)

  • Giulio Cerullo

    (Politecnico di Milano
    Istituto di Fotonica e Nanotecnologie – Consiglio Nazionale delle Ricerche)

  • Klaus Kern

    (Max Planck Institute for Solid State Research
    Ecole Polytechnique Fédérale de Lausanne)

  • Manish Garg

    (Max Planck Institute for Solid State Research)

Abstract

Probing and manipulating the spatiotemporal dynamics of hot carriers in nanoscale metals is crucial to a plethora of applications ranging from nonlinear nanophotonics to single-molecule photochemistry. The direct investigation of these highly non-equilibrium carriers requires the experimental capability of high energy-resolution (~ meV) broadband femtosecond spectroscopy. When considering the ultimate limits of atomic-scale structures, this capability has remained out of reach until date. Using a two-color femtosecond pump-probe spectroscopy, we present here the real-time tracking of hot carrier dynamics in a well-defined plasmonic picocavity, formed in the tunnel junction of a scanning tunneling microscope (STM). The excitation of hot carriers in the picocavity enables ultrafast all-optical control over the broadband (~ eV) anti-Stokes electronic resonance Raman scattering (ERRS) and the four-wave mixing (FWM) signals generated at the atomic length scale. By mapping the ERRS and FWM signals from a single graphene nanoribbon (GNR), we demonstrate that both signals are more efficiently generated along the edges of the GNR — a manifestation of atomic-scale nonlinear optical microscopy.

Suggested Citation

  • Yang Luo & Shaoxiang Sheng & Andrea Schirato & Alberto Martin-Jimenez & Giuseppe Valle & Giulio Cerullo & Klaus Kern & Manish Garg, 2025. "Visualizing hot carrier dynamics by nonlinear optical spectroscopy at the atomic length scale," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60384-2
    DOI: 10.1038/s41467-025-60384-2
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    References listed on IDEAS

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