Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics
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| Format: | Preprint |
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2026
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| _version_ | 1866908988689350656 |
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| author | Debnath, Arunangshu Mukamel, Shaul |
| author_facet | Debnath, Arunangshu Mukamel, Shaul |
| contents | In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting. This approach alleviates bottlenecks associated with probing two-exciton dynamics spread across multiple spectral and temporal windows. We demonstrate that non-classical correlations of entangled photon pairs can be used to prepare narrowband two-exciton population distributions, circumventing relaxation in mediating one-exciton states. The evolution of these population distributions and cascading optical transitions can be monitored using time-frequency-filtered two-photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to suppress or amplify specific pathways. Combining entangled photonic sources with multidimensional photon correlation spectroscopy allows promising applications in spectroscopy and sensing. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2601_20700 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics Debnath, Arunangshu Mukamel, Shaul Quantum Physics In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting. This approach alleviates bottlenecks associated with probing two-exciton dynamics spread across multiple spectral and temporal windows. We demonstrate that non-classical correlations of entangled photon pairs can be used to prepare narrowband two-exciton population distributions, circumventing relaxation in mediating one-exciton states. The evolution of these population distributions and cascading optical transitions can be monitored using time-frequency-filtered two-photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to suppress or amplify specific pathways. Combining entangled photonic sources with multidimensional photon correlation spectroscopy allows promising applications in spectroscopy and sensing. |
| title | Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics |
| topic | Quantum Physics |
| url | https://arxiv.org/abs/2601.20700 |