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Peer-reviewedCC BYThe journal of physical chemistry letters

Resolving Transient Electron-Phonon Coupling with Time-Resolved Spontaneous Raman Spectroscopy.

  • Guy Reuveni1
  • Maya Levy Greenberg1
  • Matan Menahem1
  • Olle Hellman2
  • Omer Yaffe1
  1. 1Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot76100, Israel.
  2. 2Department of Molecular Chemistry and Material Science, Weizmann Institute of Science, Rehovot76100, Israel.
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Abstract

Understanding the interaction of charge carriers with lattice vibrations in the quasi-equilibrium regime is crucial for semiconductor functionality. However, the structural signatures of these interactions are often too subtle for conventional ultrafast techniques to detect. We developed a time-resolved spontaneous Raman technique based on time-correlated single-photon counting to track the spectral response following photoexcitation, providing subwavenumber spectral resolution and a subnanosecond temporal resolution. Unlike traditional pump-probe schemes, our method utilizes a modulated continuous-wave probe to maintain high spectral resolution, enabling detection of low-frequency Raman shifts down to 10 cm-1. Applied to lightly boron-doped silicon, we resolve intra-valence band and inter-valence band electronic transitions. A coupled-mode analysis of transient phonon asymmetry, resulting from interference with the intervalence band transitions, reveals electron-phonon coupling parameters that directly relate to carrier recombination. By capturing these subtle dynamical shifts, we demonstrate that this platform offers a powerful probe for investigating electron-phonon interactions in long-lived excited states.

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Cite

BibTeXRIS
BibTeX
@article{reuveni2026resolving,
  title = {{Resolving Transient Electron-Phonon Coupling with Time-Resolved Spontaneous Raman Spectroscopy.}},
  author = {Guy Reuveni and Maya Levy Greenberg and Matan Menahem and Olle Hellman and Omer Yaffe},
  journal = {The journal of physical chemistry letters},
  year = {2026},
  month = oct,
  doi = {10.1021/acs.jpclett.6c02648},
  url = {https://europepmc.org/article/MED/42910949},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Resolving Transient Electron-Phonon Coupling with Time-Resolved Spontaneous Raman Spectroscopy.
AU  - Guy Reuveni
AU  - Maya Levy Greenberg
AU  - Matan Menahem
AU  - Olle Hellman
AU  - Omer Yaffe
PY  - 2026
DA  - 2026/10/01
JO  - The journal of physical chemistry letters
DO  - 10.1021/acs.jpclett.6c02648
UR  - https://europepmc.org/article/MED/42910949
AB  - Understanding the interaction of charge carriers with lattice vibrations in the quasi-equilibrium regime is crucial for semiconductor functionality. However, the structural signatures of these interactions are often too subtle for conventional ultrafast techniques to detect. We developed a time-resolved spontaneous Raman technique based on time-correlated single-photon counting to track the spectral response following photoexcitation, providing subwavenumber spectral resolution and a subnanosecond temporal resolution. Unlike traditional pump-probe schemes, our method utilizes a modulated continuous-wave probe to maintain high spectral resolution, enabling detection of low-frequency Raman shifts down to 10 cm-1. Applied to lightly boron-doped silicon, we resolve intra-valence band and inter-valence band electronic transitions. A coupled-mode analysis of transient phonon asymmetry, resulting from interference with the intervalence band transitions, reveals electron-phonon coupling parameters that directly relate to carrier recombination. By capturing these subtle dynamical shifts, we demonstrate that this platform offers a powerful probe for investigating electron-phonon interactions in long-lived excited states.
SN  - 1948-7185
ER  -