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| Autores principales: | , , , |
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| Formato: | Preprint |
| Publicado: |
2025
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| Materias: | |
| Acceso en línea: | https://arxiv.org/abs/2510.08809 |
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| _version_ | 1866910181986664448 |
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| author | Anwar, Tarique DallAglio, Diana Sabzehparvar, Milad Tagliabue, Giulia |
| author_facet | Anwar, Tarique DallAglio, Diana Sabzehparvar, Milad Tagliabue, Giulia |
| contents | Light and heat drive interfacial chemistry at solid-liquid interfaces, underpinning processes central to sustainable energy conversion, including photoelectrochemical and hydrovoltaic systems. Yet, non-invasive probing of light-induced interfacial dynamics remains challenging due to the weak and spatially complex nature of optical signals. Here, we introduce a nanophotonic platform that enhances second harmonic generation (SHG) from nanostructured interfaces by over two orders of magnitude, enabling real-time, all-optical access to interfacial processes. We develop a rigorous overlap-integral formalism that provides a general quantitative framework for SHG in nanostructured geometries. By accounting for spatially inhomogeneous electromagnetic fields, this approach links the nonlinear response to geometry-dependent near-field and reveals new degrees of freedom, namely independent control of attenuation and phase, which are absent in planar systems. This enables deterministic tuning of surface and electric-field-induced contributions through nanophotonic design. Using in situ SHG at silicon-oxide-electrolyte interfaces, we resolve subtle spectral shifts of ~1.3 nm with electrolyte concentration, indicating coupling between electrical double layer potential and semiconductor polarizability. Under controlled optical excitation, we observe reversible, intensity-dependent modulation of interfacial susceptibility, with a decrease at low intensities consistent with photocharging and an increase at higher intensities due to photothermal effects. These results establish nanophotonic-enhanced SHG as a quantitative and tunable probe of interfacial phenomena, providing a unified framework linking optical response, electrostatics, and geometry, and opening new avenues for controlling interfacial charge and potential with light for applications in energy conversion, catalysis, and nanophotonic devices. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_08809 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Revealing Light-Driven Dynamics at Nanostructured Solid-Liquid Interfaces with In-Situ SHG Anwar, Tarique DallAglio, Diana Sabzehparvar, Milad Tagliabue, Giulia Chemical Physics Light and heat drive interfacial chemistry at solid-liquid interfaces, underpinning processes central to sustainable energy conversion, including photoelectrochemical and hydrovoltaic systems. Yet, non-invasive probing of light-induced interfacial dynamics remains challenging due to the weak and spatially complex nature of optical signals. Here, we introduce a nanophotonic platform that enhances second harmonic generation (SHG) from nanostructured interfaces by over two orders of magnitude, enabling real-time, all-optical access to interfacial processes. We develop a rigorous overlap-integral formalism that provides a general quantitative framework for SHG in nanostructured geometries. By accounting for spatially inhomogeneous electromagnetic fields, this approach links the nonlinear response to geometry-dependent near-field and reveals new degrees of freedom, namely independent control of attenuation and phase, which are absent in planar systems. This enables deterministic tuning of surface and electric-field-induced contributions through nanophotonic design. Using in situ SHG at silicon-oxide-electrolyte interfaces, we resolve subtle spectral shifts of ~1.3 nm with electrolyte concentration, indicating coupling between electrical double layer potential and semiconductor polarizability. Under controlled optical excitation, we observe reversible, intensity-dependent modulation of interfacial susceptibility, with a decrease at low intensities consistent with photocharging and an increase at higher intensities due to photothermal effects. These results establish nanophotonic-enhanced SHG as a quantitative and tunable probe of interfacial phenomena, providing a unified framework linking optical response, electrostatics, and geometry, and opening new avenues for controlling interfacial charge and potential with light for applications in energy conversion, catalysis, and nanophotonic devices. |
| title | Revealing Light-Driven Dynamics at Nanostructured Solid-Liquid Interfaces with In-Situ SHG |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2510.08809 |