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<p>Coherent Raman scattering spectroscopies have been established as a powerful tool for investigating molecular systems with high chemical specificity. The existing coherent Raman scattering techniques detect only Raman active modes, which are a part of the whole molecular vibrations. Here, we report the first observation of coherent anti-Stokes hyper-Raman scattering (CAHRS) spectroscopy, which allows measuring hyper-Raman active vibrations at high speed. The CAHRS process relies on a fifth-order nonlinear process that combines hyper-Raman scattering with coherent Raman scattering. Observed signals are proven to come from the CAHRS process through various experiments concerning the dependences of the signals on incident laser powers, time-delay, polarizations, and selection rules of molecular vibrations. Comparisons of CAHRS signals with spontaneous hyper-Raman signals from <i>para</i>-nitroaniline solutions and benzene liquid manifest much higher signal-to-noise ratios of CAHRS signals than spontaneous hyper-Raman signals. This study illustrates that CAHRS spectroscopy can offer additional information on molecular vibrations unobtainable from the present coherent Raman techniques at a much higher speed than spontaneous hyper-Raman spectroscopy.</p>

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Coherent Anti-Stokes Hyper-Raman Spectroscopy

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月10日

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  • Kazuki Inoue,
  • Masanari Okuno

摘要

Coherent Raman scattering spectroscopies have been established as a powerful tool for investigating molecular systems with high chemical specificity. The existing coherent Raman scattering techniques detect only Raman active modes, which are a part of the whole molecular vibrations. Here, we report the first observation of coherent anti-Stokes hyper-Raman scattering (CAHRS) spectroscopy, which allows measuring hyper-Raman active vibrations at high speed. The CAHRS process relies on a fifth-order nonlinear process that combines hyper-Raman scattering with coherent Raman scattering. Observed signals are proven to come from the CAHRS process through various experiments concerning the dependences of the signals on incident laser powers, time-delay, polarizations, and selection rules of molecular vibrations. Comparisons of CAHRS signals with spontaneous hyper-Raman signals from para-nitroaniline solutions and benzene liquid manifest much higher signal-to-noise ratios of CAHRS signals than spontaneous hyper-Raman signals. This study illustrates that CAHRS spectroscopy can offer additional information on molecular vibrations unobtainable from the present coherent Raman techniques at a much higher speed than spontaneous hyper-Raman spectroscopy.