Two-colour photon correlations probe coherent vibronic contributions to
electronic excitation transport under incoherent illumination
- URL: http://arxiv.org/abs/2403.00857v1
- Date: Thu, 29 Feb 2024 19:00:05 GMT
- Title: Two-colour photon correlations probe coherent vibronic contributions to
electronic excitation transport under incoherent illumination
- Authors: Charlie Nation, Valentina Notararigo, Hallmann Oskar Gestsson, Luca
Sapienza, Alexandra Olaya-Castro
- Abstract summary: We consider a prototype light-harvesting heterodimer exhibiting coherent and collective exciton-vibration interactions.
We show that coherent vibronic mechanisms strongly affect the asymmetries characteristic of time-resolved photon cross-correlations.
We discuss how such second-order correlation asymmetry establishes important connections between coherent vibronic interactions, directional exciton population transport, and violation of quantum detailed balance.
- Score: 41.94295877935867
- License: http://creativecommons.org/licenses/by/4.0/
- Abstract: Identifying signatures of quantum coherent behaviour in photoactive systems
that are maintained in stationary states away from thermal equilibrium is an
open problem of wide interest in a variety of physical scenarios, including
single photosynthetic complexes subjected to continuous incoherent
illumination. Here we consider a prototype light-harvesting heterodimer
exhibiting coherent and collective exciton-vibration interactions and show that
the second-order frequency-filtered correlations of fluorescence photons
provide insightful information on the influence of such coherent interactions
for different transitions, thereby yielding fundamentally different
photon-counting statistics. Furthermore, we show that coherent vibronic
mechanisms strongly affect the asymmetries characteristic of time-resolved
photon cross-correlations and manifest themselves in a time-dependent violation
of the Cauchy-Schwarz inequality bounding cross-correlations for classically
fluctuating fields. We finally discuss how such second-order correlation
asymmetry establishes important connections between coherent vibronic
interactions, directional exciton population transport, and violation of
quantum detailed balance. Our work then indicates that measurement of
two-colour photon correlation asymmetry can be an important avenue to
investigate quantum behaviour of single photoactive biomolecular and chemical
systems under incoherent illumination conditions.
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