Mapping molecular polariton transport via pump-probe microscopy
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arXiv
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| Format: | Preprint |
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2025
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| _version_ | 1866914578687852544 |
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| author | Fowler-Wright, Piper Reitz, Michael Yuen-Zhou, Joel |
| author_facet | Fowler-Wright, Piper Reitz, Michael Yuen-Zhou, Joel |
| contents | We demonstrate how the transport properties of molecular polaritons in optical cavities can be extracted from a microscopic modeling of pump-probe spectroscopy. Our approach combines a mean-field treatment of the light-matter Hamiltonian with a perturbative expansion of both light and matter components, along with spatial coarse-graining. This approach extends semiclassical cavity spectroscopy to multimode light-matter interactions, providing full access to spatially resolved transient spectra. By simulating a microscopy experiment with counter-propagating pump and probe pulses, we compute the differential transmission and show how molecular dephasing and persistent dark exciton populations drive sub-group-velocity transport of the root-mean-square displacement. We analyze transport across the polariton dispersion, showing how velocity renormalization correlates with excitonic weight, consistent with experimental observations, and further its dependence on the rate of molecular dephasing. Our results highlight the need to consider measured spectroscopic observables when characterizing transport in polaritonic systems. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2504_15501 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Mapping molecular polariton transport via pump-probe microscopy Fowler-Wright, Piper Reitz, Michael Yuen-Zhou, Joel Quantum Physics Mesoscale and Nanoscale Physics Chemical Physics Optics We demonstrate how the transport properties of molecular polaritons in optical cavities can be extracted from a microscopic modeling of pump-probe spectroscopy. Our approach combines a mean-field treatment of the light-matter Hamiltonian with a perturbative expansion of both light and matter components, along with spatial coarse-graining. This approach extends semiclassical cavity spectroscopy to multimode light-matter interactions, providing full access to spatially resolved transient spectra. By simulating a microscopy experiment with counter-propagating pump and probe pulses, we compute the differential transmission and show how molecular dephasing and persistent dark exciton populations drive sub-group-velocity transport of the root-mean-square displacement. We analyze transport across the polariton dispersion, showing how velocity renormalization correlates with excitonic weight, consistent with experimental observations, and further its dependence on the rate of molecular dephasing. Our results highlight the need to consider measured spectroscopic observables when characterizing transport in polaritonic systems. |
| title | Mapping molecular polariton transport via pump-probe microscopy |
| topic | Quantum Physics Mesoscale and Nanoscale Physics Chemical Physics Optics |
| url | https://arxiv.org/abs/2504.15501 |