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

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Main Authors: Reuveni, Guy, Greenberg, Maya Levy, Menahem, Matan, Hellman, Olle, Yaffe, Omer
Format: Preprint
Published: 2026
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_version_ 1866911503264776192
author Reuveni, Guy
Greenberg, Maya Levy
Menahem, Matan
Hellman, Olle
Yaffe, Omer
author_facet Reuveni, Guy
Greenberg, Maya Levy
Menahem, Matan
Hellman, Olle
Yaffe, Omer
contents 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 sub-wavenumber spectral resolution and a few-hundred-picosecond 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 inter-valence 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.
format Preprint
id arxiv_https___arxiv_org_abs_2603_09755
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Resolving Transient Electron-Phonon Coupling with Time-Resolved Spontaneous Raman Spectroscopy
Reuveni, Guy
Greenberg, Maya Levy
Menahem, Matan
Hellman, Olle
Yaffe, Omer
Materials Science
Optics
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 sub-wavenumber spectral resolution and a few-hundred-picosecond 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 inter-valence 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.
title Resolving Transient Electron-Phonon Coupling with Time-Resolved Spontaneous Raman Spectroscopy
topic Materials Science
Optics
url https://arxiv.org/abs/2603.09755