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Selective excitation of vibrations in a single molecule

Author

Listed:
  • Yang Luo

    (Max Planck Institute for Solid State Research)

  • Shaoxiang Sheng

    (Max Planck Institute for Solid State Research)

  • Michele Pisarra

    (Università della Calabria
    Gruppo Collegato di Cosenza)

  • Alberto Martin-Jimenez

    (Max Planck Institute for Solid State Research
    Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nano), Faraday 9, Cantoblanco)

  • Fernando Martin

    (Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nano), Faraday 9, Cantoblanco
    Universidad Autónoma de Madrid)

  • Klaus Kern

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

  • Manish Garg

    (Max Planck Institute for Solid State Research)

Abstract

The capability to excite, probe, and manipulate vibrational modes is essential for understanding and controlling chemical reactions at the molecular level. Recent advancements in tip-enhanced Raman spectroscopies have enabled the probing of vibrational fingerprints in a single molecule with Ångström-scale spatial resolution. However, achieving controllable excitation of specific vibrational modes in individual molecules remains challenging. Here, we demonstrate the selective excitation and probing of vibrational modes in single deprotonated phthalocyanine molecules utilizing resonance Raman spectroscopy in a scanning tunneling microscope. Selective excitation is achieved by finely tuning the excitation wavelength of the laser to be resonant with the vibronic transitions between the molecular ground electronic state and the vibrational levels in the excited electronic state, resulting in the state-selective enhancement of the resonance Raman signal. Our approach contributes to setting the stage for steering chemical transformations in molecules on surfaces by selective excitation of molecular vibrations.

Suggested Citation

  • Yang Luo & Shaoxiang Sheng & Michele Pisarra & Alberto Martin-Jimenez & Fernando Martin & Klaus Kern & Manish Garg, 2024. "Selective excitation of vibrations in a single molecule," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51419-1
    DOI: 10.1038/s41467-024-51419-1
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    References listed on IDEAS

    as
    1. R. Zhang & Y. Zhang & Z. C. Dong & S. Jiang & C. Zhang & L. G. Chen & L. Zhang & Y. Liao & J. Aizpurua & Y. Luo & J. L. Yang & J. G. Hou, 2013. "Chemical mapping of a single molecule by plasmon-enhanced Raman scattering," Nature, Nature, vol. 498(7452), pages 82-86, June.
    2. Yang Luo & Alberto Martin-Jimenez & Michele Pisarra & Fernando Martin & Manish Garg & Klaus Kern, 2023. "Imaging and controlling coherent phonon wave packets in single graphene nanoribbons," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Joonhee Lee & Kevin T. Crampton & Nicholas Tallarida & V. Ara Apkarian, 2019. "Visualizing vibrational normal modes of a single molecule with atomically confined light," Nature, Nature, vol. 568(7750), pages 78-82, April.
    4. Shahnawaz R. Rather & Nicholas P. Weingartz & Sarah Kromer & Felix N. Castellano & Lin X. Chen, 2023. "Spin–vibronic coherence drives singlet–triplet conversion," Nature, Nature, vol. 620(7975), pages 776-781, August.
    5. J. I. Pascual & N. Lorente & Z. Song & H. Conrad & H.-P. Rust, 2003. "Selectivity in vibrationally mediated single-molecule chemistry," Nature, Nature, vol. 423(6939), pages 525-528, May.
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