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.
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.
In this thesis a formalism for indistinguishable multi-level quantum emitters in quantum master equations is developed. The complexity of the approach scales only polynomially in the number of quantum emitters. Complexity here means the number of coupled equations or rather the dimension of the Liouville space. This approach opens new possibilities for calculating open quantum systems. The method is implemented in the PsiQuaSP library, which allows to setup and solve arbitrary master equations, in particular master equations with the reduced polyno-mial scaling. The introduced tools are utilized to study subradiance in the open Dicke model and various cQED lasers. One of the main current research goals in quantum optics and quantum information science is the generation and stabilization of quantum coherence between distinct quantum systems. These systems can for instance be photons or quantum emitters, qubits. From a theoretical stance the difficulty with these systems is that their complexity scales in general exponentially with the system size, like the number of quantum emitters. The reduced scaling of the formalism introduced in this thesis stems from the permutation symmetry of the indistinguishable emitters. The method is derived in the context of Lindblad quantum master equations. Lindblad quantum master equations for many identical multi-level systems have been used to study funda- mental quantum optical systems, such as lasing and laser like action, various phase transitions, optical bistability, cooperative resonance fluorescence, entanglement, quantum light generation, quantum to classical transitions, super- and subradiance etc. In most of these cases the single emitter, the many emitter and the weak correlation limit can be satisfactorily treated with existing techniques, such as direct integration, phase space methods or cluster expansion. However these techniques are not well suited for the few emitter case with strong correlations. The theory developed in this thesis allows to study all these systems for moderate numbers of quantum emitters and arbitrary correlation strengths, thus filling the gap left open by conventional methods. Even though the theory is developed around Lindblad quantum master equations it is not limited to this case – the requirement of indistinguishability is used to construct symmetrized Liouville space basis states and operators which can also be used to construct other master equations. In this thesis the general methodology for the polynomial scaling of the many emitter master equation is derived by two different approaches. Generalized permutation symmetric Liouville space states and operators are introduced that allow for the construction of arbitrary master equations and observables. These Liouville space states and operators are translated into a graphical representation that greatly facilitates their usage. This representation is found to have a close connection to Lie algebras as well as graph theory. The whole method is implemented in a general and modular way in a C++ library called PsiQuaSP, which allows to simulate arbitrary master equations based on a number state representation. The design of the library heavily relies on the introduced graphical representation, which greatly facilitates the setup of a simulation. The treatment of non-identical systems with PsiQuaSP is illustrated and further techniques for complexity reduction and computational speedup are discussed. These tools are applied to the two main cases of cQED lasers/spasers and super-, subradiance. In the latter case a new type of phase transition in the open Dicke model is predicted that leads to a deterministic generation of subradiant steady state coherences, with applications in quantum information science. Furthermore the interaction of quantum dots with the dissipative modes at metal interfaces is investigated in order to explain experimental findings.
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 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.
Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative aspects such as dipole-dipole interactions and subradiance find applications in the design of nanoscale coherent light sources and highly-reflective quantum metasurfaces made up of hundreds of optically trapped atoms, in the implementation of topological quantum optics on subwavelength arrays of emitters, in quantum metrology and quantum information. The quick bursts of radiation from a collection of quasi-indistiguishable emitters provides an alternative approach to standard lasers by introducing superradiant lasers operating at extremely low intracavity power. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity in light-matter systems by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitters ensembles. These analytical approaches are then also extended to frequency disordered or vibronically coupled quantum emitter ensembles with wide relevance ranging from atoms in optical lattices, quantum dots in solid state environments or molecular quantum systems.
Reduced abstract. This Thesis explores emergent cooperative phenomena in collective light-matter systems. We study ensembles of interacting quantum emitters coherently driven by a laser field and coupled to photonic structures, focusing on the hybrid description of emitters dressed by light. The interplay among quantum emitters, coherent driving, and photonic environments reveals a rich landscape of cooperative effects. While single-emitter dressing has been widely studied, we address collective phenomena in two non-identical emitters modelled as two-level systems. Strong interaction forms a dimer exhibiting superradiant and subradiant states, with two-photon resonances directly connecting ground and doubly excited states. This nonlinear process, central to the Thesis, enables new regimes of cooperative light-matter physics. Analytical studies show how interactions reshape observables such as emission intensity, photon statistics, and spectra, offering implications for quantum metrology. The sensitivity of two-photon processes to emitter distance and driving strength enables high-precision sensing and sub-wavelength imaging. Unexpectedly, we find that off-resonant virtual states may gain population through dissipation, redefining their role in open systems. To capture this, we develop a hierarchical adiabatic elimination method for metastable dynamics. We also analyze entanglement in emitters coupled to a lossy cavity, identifying five mechanisms, including the frequency-resolved Purcell effect introduced here. This selective enhancement stabilizes cooperative states and enables scalable entanglement. Our models, tailored to solid-state platforms such as quantum dots and molecular aggregates, address challenges like inhomogeneous broadening and decoherence, demonstrating the feasibility of harnessing cooperative light-matter effects for quantum technologies.
We obtained the system of Maxwell-Bloch equations (MB) that describe the interaction of cw laser with optically active impurity centers (particles) embedded in a dielectric material. The dielectric material is considered as a continuous medium with sufficient laser detuning from its absorption lines. The model takes into account the effects associated with both the real and the imaginary part of the dielectric constant of the material. MB equations were derived within a many-particle quantum-kinetic formalism, which is based on Bogolyubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy for reduced density matrices and correlation operators of material particles and the quantized radiation field modes. It is shown that this method is beneficial to describe the effects of individual and collective behavior of the light emitters and requires no phenomenological procedures. It automatically takes into account the characteristics associated with the presence of non-resonant and resonant particles filling the space between the optical centers.