Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics
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 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.
Keywords
Cite
@article{arxiv.2601.20700,
title = {Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics},
author = {Arunangshu Debnath and Shaul Mukamel},
journal= {arXiv preprint arXiv:2601.20700},
year = {2026}
}
Comments
Submitted 14/04/2025 (under review)