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Sub-optical-cycle light-matter energy transfer in molecular vibrational spectroscopy

Author

Listed:
  • Martin T. Peschel

    (Ludwig-Maximilians-Universität München)

  • Maximilian Högner

    (Max-Planck-Institut für Quantenoptik
    Ludwig-Maximilians-Universität München)

  • Theresa Buberl

    (Max-Planck-Institut für Quantenoptik
    Ludwig-Maximilians-Universität München)

  • Daniel Keefer

    (Ludwig-Maximilians-Universität München
    University of California)

  • Regina Vivie-Riedle

    (Ludwig-Maximilians-Universität München)

  • Ioachim Pupeza

    (Max-Planck-Institut für Quantenoptik
    Ludwig-Maximilians-Universität München)

Abstract

The evolution of ultrafast-laser technology has steadily advanced the level of detail in studies of light-matter interactions. Here, we employ electric-field-resolved spectroscopy and quantum-chemical modelling to precisely measure and describe the complete coherent energy transfer between octave-spanning mid-infrared waveforms and vibrating molecules in aqueous solution. The sub-optical-cycle temporal resolution of our technique reveals alternating absorption and (stimulated) emission on a few-femtosecond time scale. This behaviour can only be captured when effects beyond the rotating wave approximation are considered. At a femtosecond-to-picosecond timescale, optical-phase-dependent coherent transients and the dephasing of the vibrations of resonantly excited methylsulfonylmethane (DMSO2) are observed. Ab initio modelling using density functional theory traces these dynamics back to molecular-scale sample properties, in particular vibrational frequencies and transition dipoles, as well as their fluctuation due to the motion of DMSO2 through varying solvent environments. Future extension of our study to nonlinear interrogation of higher-order susceptibilities is fathomable with state-of-the-art lasers.

Suggested Citation

  • Martin T. Peschel & Maximilian Högner & Theresa Buberl & Daniel Keefer & Regina Vivie-Riedle & Ioachim Pupeza, 2022. "Sub-optical-cycle light-matter energy transfer in molecular vibrational spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33477-5
    DOI: 10.1038/s41467-022-33477-5
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    References listed on IDEAS

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    1. Ioachim Pupeza & Marinus Huber & Michael Trubetskov & Wolfgang Schweinberger & Syed A. Hussain & Christina Hofer & Kilian Fritsch & Markus Poetzlberger & Lenard Vamos & Ernst Fill & Tatiana Amotchkina, 2020. "Field-resolved infrared spectroscopy of biological systems," Nature, Nature, vol. 577(7788), pages 52-59, January.
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