Entangled biphoton enhanced double quantum coherence signal as a probe for cavity polariton correlations in presence of phonon induced dephasing

TL;DR

This paper proposes a biphoton entanglement-enhanced spectroscopic technique to probe cavity polariton dynamics and correlations in photosynthetic complexes, effectively capturing ultrafast dephasing effects and exciton migration.

Contribution

It introduces a novel biphoton-based spectroscopic method that is highly sensitive to polariton coherence and excitonic correlations under dissipative conditions.

Findings

Enhanced sensitivity to inter-manifold polariton coherence.

Ability to monitor cavity-mediated excitonic correlations.

Detection of long-range cavity-assisted exciton migration.

Abstract

We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic complex that represents a prototypical multi-site excitonic quantum aggregate. The proposed technique is shown to be particularly sensitive to inter-manifold polariton coherence between the two and one-excitation subspaces. It is demonstrated to be able to monitor the dynamical role of cavity-mediated excitonic correlations, and dephasing in the presence of phonon-induced dissipation. The non-classicality of the entangled biphoton sources is shown to enhance the ultra-fast and broadband correlation features of the signal, giving an indication about the underlying state correlations responsible for long-range cavity-assisted exciton migration.