Photon correlation time-asymmetry and dynamical coherence in multichromophoric systems

• URL: http://arxiv.org/abs/2404.16892v1
• Date: Wed, 24 Apr 2024 21:06:01 GMT
• Title: Photon correlation time-asymmetry and dynamical coherence in multichromophoric systems
• Authors: Charlie Nation, Hallmann Oskar Gestsson, Alexandra Olaya-Castro,
• Abstract summary: We show that time-asymmetries in the cross-correlations of photons corresponding to different polarizations can be exploited to probe quantum coherent transport mechanisms and steady-state coherence properties. Our results put forward photon correlation asymmetry as a promising approach to investigate coherent contributions to excited-stated dynamics in molecular aggregates and other many-site quantum emitters.
• Score: 44.99833362998488
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We theoretically investigate polarization-filtered two-photon correlations for the light emitted by a multichromophoric system undergoing excitation transport under realistic exciton-phonon interactions, and subject to continuous incoherent illumination. We show that for a biomolecular aggregate, such as the Fenna-Matthews Olson (FMO) photosynthetic complex, time-asymmetries in the cross-correlations of photons corresponding to different polarizations can be exploited to probe both quantum coherent transport mechanisms and steady-state coherence properties, which are not witnessed by zero-delay correlations. A classical bound on correlation asymmetry is obtained, which FMO is shown to violate using exact numerical calculations. Our analysis indicates that the dominant contributions to time-asymmetry in such photon cross-correlations are population to coherence transfer for Frenkel-Exciton models. Our results therefore put forward photon correlation asymmetry as a promising approach to investigate coherent contributions to excited-stated dynamics in molecular aggregates and other many-site quantum emitters.

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