Broadband ultrafast self-heterodyned chiro-optical spectroscopy
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arXiv
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| Autores principales: | , , , , , , , , , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2025
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| _version_ | 1866911263879069696 |
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| author | Gucci†, Francesco Iudica†, Andrea Tacchi†, Andres Valladares Y Schirato, Andrea Crotti, Giulia Kim, Ryeong Myeong Lee, Soo Min Han, Jeong Hyun Villa, Andrea Ali, Dawar Rizzo, Aurora Maiuri, Margherita Nam, Ki Tae Della Valle, Giuseppe Cerullo, Giulio |
| author_facet | Gucci†, Francesco Iudica†, Andrea Tacchi†, Andres Valladares Y Schirato, Andrea Crotti, Giulia Kim, Ryeong Myeong Lee, Soo Min Han, Jeong Hyun Villa, Andrea Ali, Dawar Rizzo, Aurora Maiuri, Margherita Nam, Ki Tae Della Valle, Giuseppe Cerullo, Giulio |
| contents | Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 $μ$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2511_10574 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Broadband ultrafast self-heterodyned chiro-optical spectroscopy Gucci†, Francesco Iudica†, Andrea Tacchi†, Andres Valladares Y Schirato, Andrea Crotti, Giulia Kim, Ryeong Myeong Lee, Soo Min Han, Jeong Hyun Villa, Andrea Ali, Dawar Rizzo, Aurora Maiuri, Margherita Nam, Ki Tae Della Valle, Giuseppe Cerullo, Giulio Optics Other Condensed Matter Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 $μ$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics. |
| title | Broadband ultrafast self-heterodyned chiro-optical spectroscopy |
| topic | Optics Other Condensed Matter |
| url | https://arxiv.org/abs/2511.10574 |