Optical signatures of coherence in molecular dimers

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Abstract

We calculate experimentally measurable signatures of quantum correlations in a coupled molecular dimer that strongly interacts with its vibrational environment. We investigate intensity and mode-resolved photon coincidences for different relative orientations of such dimers and observe spatio-temporal correlations for various configurations. We find that projective measurements can produce cooperative signatures even when emitters are arranged orthogonal to each other. To model effects of vibrational environments that are present in realistic experimental situations, we use the polaron framework. Furthermore, we also account for the effects of finite instrument response, varying temperature, and the presence of static disorder. We analyze the effect of disorder in both dimer orientation and measurement direction and find that photon coincidences remain well-resolvable using state-of-the-art detectors. This work enhances our understanding of cooperative emission from two coupled emitters and offers direction for future experiments on probing their coherent dynamics.
Original languageEnglish
Article number204103
JournalJournal of Chemical Physics
Volume163
Issue number20
Early online date24 Nov 2025
DOIs
Publication statusPublished - 28 Nov 2025

Keywords

  • Excitons
  • Phonons
  • Polarons
  • Direction finding
  • Quantum correlations
  • Dark states
  • Photoemission
  • Quantum coherence
  • Cooperative effect

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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