Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics

• URL: http://arxiv.org/abs/2601.20700v2
• Date: Thu, 05 Feb 2026 18:58:29 GMT
• Title: Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics
• Authors: Arunangshu Debnath, Shaul Mukamel,
• Abstract summary: We propose a protocol that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting.<n>We demonstrate that non-classical correlations of entangled photon pairs can be used to prepare narrowband two-exciton population distributions.<n>The evolution of these population distributions and cascading transitions can be monitored using time-frequency-filtered photon coincidence counting.
• Score: 0.0
• License: http://creativecommons.org/licenses/by-nc-nd/4.0/
• Abstract: 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 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, thereby circumventing transport in mediating one-exciton states. The evolution of these population distributions and cascading transitions can be monitored using time-frequency-filtered photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to achieve selectivity by suppressing or amplifying specific pathways. Combining entangled photonic sources with multidimensional photon counting allows promising applications in spectroscopy and sensing.

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