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Bulletin of the Russian Academy of Sciences Physics

Theoretical Modeling of Superradiant and Subradiant Photoluminescence in Pairs of Lifetime-Limited Organic Molecules

Ekaterina A. Tarasevich, V. D. Burova, М. Г. Гладуш

Published Dec 1, 2025• 0 citations
Publisher

Abstract

Abstract We present numerical calculations of the cooperative photoluminescence spectra of two dipole–dipole–coupled dibenzoterrylene molecules embedded in an anthracene crystal at liquid-helium temperature. Using master-equation formalism for non-identical two-level emitters, we reproduce the excitation spectra recently observed in experiment. The excellent agreement between the simulations, analytical model, and measurements confirms the observation of controllable molecular entanglement and validates the theoretical framework. The approach provides an efficient computational tool for predicting and controlling cooperative photoluminescence in solid-state molecular systems. These results establish a basis for future experiments aimed at achieving optical entanglement of organic molecules and developing quantum photonic devices.

DOI
10.1134/s1062873825715016

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Abstract We present numerical calculations of the cooperative photoluminescence spectra of two dipole–dipole–coupled dibenzoterrylene molecules embedded in an anthracene crystal at liquid-helium temperature. Using master-equation formalism for non-identical two-level emitters, we reproduce the excitation spectra recently observed in experiment. The excellent agreement between the simulations, analytical model, and measurements confirms the observation of controllable molecular entanglement and validates the theoretical framework. The approach provides an efficient computational tool for predicting and controlling cooperative photoluminescence in solid-state molecular systems. These results establish a basis for future experiments aimed at achieving optical entanglement of organic molecules and developing quantum photonic devices.
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The applicability of the method for measuring the probe absorption and gain spectra in a system of quantum emitters excited by a resonant driving field for studying cooperative photoluminescence is considered. The gain and attenuation of a probe signal in the system of two quantum emitters with the dipole–dipole interaction have been calculated for the conditions of observing the cooperative photoluminescence of a pair of impurity molecules described in the literature and close to them. The resulting dependences demonstrate the structure of excited collective molecular states, which can be used to reconstruct the positions of molecules in a matrix and to determine the difference in their photophysical properties. Thus, the probe absorption and gain spectra can be used to analyze the photoluminescence of quantum-entangled particles and to transform light signals.
Abstract An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes, and second-order correlation agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in sub-wavelength arrays of quantum emitters.
Whether many-body objects like organic molecules can exhibit full quantum behaviour, including entanglement, is an open fundamental question. We present a generic theoretical protocol for entangling two organic molecules, such as dibenzoterrylene in anthracene. The availability of organic dye molecules with two-level energy structures characterised by sharp and intense emission lines are characteristics that position them favourably as candidates for quantum information processing technologies involving single-photons. Quantum entanglement can in principle be generated between several organic molecules by carefully interfering their photoluminescence spectra. Major milestones have been achieved in the last 10 years showcasing entanglement in diverse systems including ions, cold atoms, superconductors, photons, quantum dots and NV-centres in diamond, but not yet in molecules.
We report progress in the theory of photoluminescence and light scattering by two closely spaced particles. This study is based on our original method to derive the master equation for a system of coupled quantum emitters driven by a cw laser. We emphasise on the case when the emitters are two-level systems but notably different in their transition frequencies and transition moments. The master equation is shown to describe the dipole-dipole coupling and the cooperative entanglement between the particles naturally. It is provided by the use of the Bogolyubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchies for reduced density matrices and correlation operators of the material and photonic subsystems. Tackling the hierarchies has also provided us with an elegant way to calculate the photoluminescence excitation spectra subject to the arrangement of the excitation and the position of the detector against the emitters. Our findings may be important for developing novel possibilities for the all-optical nanoscopy and may help construction of entangled systems to be implemented in quantum technologies.
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