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| Main Authors: | , , , , , , , |
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| Format: | Preprint |
| Published: |
2026
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2603.01442 |
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| _version_ | 1866917305448923136 |
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| author | Sugimoto, Toshiki Ichii, Tomoaki Kanai, Tsuneto Yoshizawa, Ryu Takahashi, Shota Sakurai, Atsunori Seto, Keisuke Chengxiang, Jin |
| author_facet | Sugimoto, Toshiki Ichii, Tomoaki Kanai, Tsuneto Yoshizawa, Ryu Takahashi, Shota Sakurai, Atsunori Seto, Keisuke Chengxiang, Jin |
| contents | Coherent Raman scattering provides highly sensitive vibrational analysis through nonlinear light-matter interactions. However, its application to metal interfaces has remained challenging because the intrinsically large non-resonant background (NRB) of metals overwhelms weak interfacial molecular vibrational signals, making direct Raman detection without plasmonic or electronic enhancement highly challenging. Here, we report a time-frequency hybrid coherent Raman spectroscopy approach that overcomes this limitation and enables sensitive detection of ångström-thick molecular systems even on atomically flat metal surfaces. Our method employs a time-frequency engineered detection scheme that combines femtosecond pump and Stokes pulses with a time-delayed, asymmetrically shaped picosecond probe pulse. By exploiting instantaneous temporal response of the metal NRB, this pulse configuration effectively filters out the dominant metal NRB in the time domain while retaining a controlled residual NRB that acts as an internal local oscillator, enabling strong interferometric amplification of weak interfacial vibrational signatures. This all-optical coherent enhancement strategy establishes a new route for direct, non-invasive Raman detection of interfacial molecular systems across a wide range of surfaces without requiring structure- and material-specific plasmonic and electronic enhancement mechanisms. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2603_01442 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Plasmonic- and Electronic-Enhancement-Free Coherent Raman Detection of Ångström-Scale Molecular Layers at Metal Interfaces Sugimoto, Toshiki Ichii, Tomoaki Kanai, Tsuneto Yoshizawa, Ryu Takahashi, Shota Sakurai, Atsunori Seto, Keisuke Chengxiang, Jin Optics Materials Science Coherent Raman scattering provides highly sensitive vibrational analysis through nonlinear light-matter interactions. However, its application to metal interfaces has remained challenging because the intrinsically large non-resonant background (NRB) of metals overwhelms weak interfacial molecular vibrational signals, making direct Raman detection without plasmonic or electronic enhancement highly challenging. Here, we report a time-frequency hybrid coherent Raman spectroscopy approach that overcomes this limitation and enables sensitive detection of ångström-thick molecular systems even on atomically flat metal surfaces. Our method employs a time-frequency engineered detection scheme that combines femtosecond pump and Stokes pulses with a time-delayed, asymmetrically shaped picosecond probe pulse. By exploiting instantaneous temporal response of the metal NRB, this pulse configuration effectively filters out the dominant metal NRB in the time domain while retaining a controlled residual NRB that acts as an internal local oscillator, enabling strong interferometric amplification of weak interfacial vibrational signatures. This all-optical coherent enhancement strategy establishes a new route for direct, non-invasive Raman detection of interfacial molecular systems across a wide range of surfaces without requiring structure- and material-specific plasmonic and electronic enhancement mechanisms. |
| title | Plasmonic- and Electronic-Enhancement-Free Coherent Raman Detection of Ångström-Scale Molecular Layers at Metal Interfaces |
| topic | Optics Materials Science |
| url | https://arxiv.org/abs/2603.01442 |