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

TL;DR

This paper introduces a novel spectroscopy protocol using entangled photons and time-frequency filtering to probe exciton dynamics in molecular aggregates with high spectral and temporal resolution.

Contribution

It combines photon-entanglement-enhanced excitation with time-frequency-filtered coincidence counting to improve the monitoring of two-exciton state dynamics.

Findings

Demonstrates suppression or amplification of specific pathways in simulations.

Shows non-classical correlations can prepare narrowband two-exciton populations.

Highlights potential for advanced spectroscopy and sensing applications.

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.