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.
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.
The interaction between light and matter has captivated physicists for centuries, from early studies of vision and refraction in ancient Greece to the development of quantum mechanics and quantum electrodynamics in the past century. While the response of a single quantum emitter to light is well understood, the radiative properties of an ensemble of closely spaced emitters are far more intricate. Coupling to a shared electromagnetic environment induces coherent and dissipative interactions between emitters, giving rise to a collective response that cannot be captured by treating them independently. In the regime of few excitations, the system hosts delocalized subradiant states, that is, coherent superpositions that are largely decoupled from the electromagnetic field and thus decay at suppressed rates. While this weak coupling makes subradiant states attractive for quantum technologies, it also renders them difficult to manipulate. At higher excitation densities, the intrinsic nonlinearity of emitters and the exponential growth of the Hilbert space make theoretical and numerical descriptions of the system and its dynamics increasingly challenging. This thesis explores two fundamental questions: How can subradiant and dark states be selectively accessed and harnessed for practical applications in quantum technologies? And how can interacting ensembles of quantum emitters be efficiently simulated to uncover their many-body physics? The first part of the thesis develops protocols for controlling and addressing dark states in free-space and waveguide-coupled atomic arrays, demonstrating their utility in quantum storage and the deterministic generation of entangled photonic states. Incorporating atomic motion, we further show that collective subradiant states can enhance cooling in dense atomic arrays, offering new avenues for controlling motional dynamics. In the second part, we introduce cumulant expansions of the equations of motion as a powerful tool to analytically and numerically investigate collective decay in the many-body regime. We first examine the collective decay of fully excited atomic arrays in free space, characterizing the onset and scaling of the superradiant burst across different geometries. In collaboration with experiments on ultracold erbium atoms in optical lattices, we provide the first direct observations of many-body collective effects in free-space ordered arrays, including early-time superradiant bursts, late-time subradiant tails, and the emergence of atomic correlations throughout the dynamics. Finally, we theoretically and numerically explore the transient formation of multi-excitation subradiant states, and demonstrate how the existence of multiple dissipation channels suppresses steady-state superradiance in extended arrays.
Two nonidentical quantum emitters, when placed within a cavity and coherently excited at the two-photon resonance, can reach stationary states of nearly maximal entanglement. In Vivas-Viaña, Martín-Cano, and Sánchez Muñoz [], we introduce a frequency-resolved Purcell effect stabilizing entangled W states among strongly interacting quantum emitters embedded in a cavity. Here we delve deeper into a specific configuration with a particularly rich phenomenology: two interacting quantum emitters under coherent excitation at the two-photon resonance. This scenario yields two resonant cavity frequencies where the combination of two-photon driving and Purcell-enhanced decay stabilizes the system into the subradiant and superradiant states, respectively. By considering the case of nondegenerate emitters and exploring the parameter space of the system, we show that this mechanism is merely one among a complex family of phenomena that can generate both stationary and metastable entanglement when driving the emitters at the two-photon resonance. We provide a global perspective of this landscape of mechanisms and contribute analytical characterizations and insights into these phenomena, establishing connections with previous reports in the literature and discussing how some of these effects can be optically detected. Published by the American Physical Society 2024
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.
Quantum mechanics is fundamentally governed by the Schrödinger equation, which is linear in the wave function. Nevertheless, quantum systems can exhibit highly nonlinear behavior in their observable dynamics. Such nonlinearities can emerge from many-body interactions, nonlinear coupling mechanisms, or the interplay between coherent evolution and dissipation. In the collective limit, microscopic quantum interactions can give rise to qualitatively new macroscopic behavior. Open quantum systems provide a rich setting for such phenomena, as environmental coupling introduces dissipation and fluctuations that compete with coherent dynamics and can alter the steady states and dynamical phases of a system. Combined with nonlinear interactions, this competition can produce behavior with no direct counterpart in conventional linear light--matter systems. In this thesis, I investigate such collective phenomena through nonlinear two-photon light--matter interactions and engineered quantum reservoirs. I first investigate the driven--dissipative two-photon Dicke model and demonstrate the emergence of a dissipative superradiant phase transition. The quadratic light--matter interaction introduces distinct stability requirements in the presence of dissipation. In particular, two-photon loss stabilizes the superradiant phase, allowing its steady states and critical behavior to be characterized. I next investigate photon blockade and transient quadrature-squeezed radiation in the two-photon Tavis--Cummings model. I show that two-photon interactions collectively enhance photon blockade and squeezing, in contrast to the conventional one-photon model, where the effective nonlinearity diminishes in the collective limit. Finally, I consider collective behavior induced by reservoir engineering. Two spatially separated open quantum systems without direct coherent interaction can undergo a nonlocal quantum phase transition when coupled to correlated quantum reservoirs. Remarkably, the transition is hidden from local observables and emerges only through nonlocal correlations and collective observables. Together, these results demonstrate how nonlinear interactions and engineered dissipation can reshape collective behavior in open quantum systems.
Multi-photon lasing has been realized in systems with strong nonlinear interactions between emitters and cavity modes, where single-photon processes are suppressed. Coherence between the internal states of a quantum emitter, or among multiple emitters, plays a key role. Such continuous nonclassical sources of light can find applications in quantum computation, quantum sensing, quantum metrology, and quantum communication.
This thesis explores the multi-photon lasing phenomena in various quantum dot-photonic crystal cavity quantum electrodynamic (QED) setups. Exciton-phonon interactions are inevitable in such systems and are incorporated using the polaron-transformed master equation. The Born-Markov approximation is employed to obtain the reduced density matrix rate equation. Using quantum laser theory, we derived the Scully-Lamb laser rate equations and evaluated the single- and multi-photon excess emission rates defined as the difference between emission and absorption rates into the cavity mode without mean-field approximations. We investigated cooperative two-photon lasing, correlated emission lasing, hyperradiant lasing, non-degenerate two-mode two-photon lasing, and continuous variable entanglement in open quantum systems with single or multiple semiconductor quantum dots (two-level, three-level, and four-level) driven coherently/incoherently and coupled to single/ bimodal cavities.
In recent years, the study of quantum electrodynamics (QED) in light-matter interactions has discovered various interesting phenomenons that orient many applications. However, due to the ambient entanglement among photons and atoms, few-particle dynamics remains challenging to analyze precisely and limits the progress in several fields. In few-particle systems, different number of atoms interacting with the light field generates drastically different results, even when there is only a single photon involved in the system. The interference between individual atom’s spontaneous emission wavefunctions can cooperatively alter the effective atom-light coupling strength. Depending on the spatial distance between individual of atoms and the involved cavities in the interaction progresses, the collective spontaneous emission rate can alter drastically from superradiance, where the emission rate is enhanced to a high value proportional to the atom number, to subradiance, where the excited atom ensemble stays in a dark state with the light trapped forever. Superradiance provides a promising mechanism to create an ultra-strong light-matter coupling environment, which is an important ingredient for the design of ultra-fast optical devices, frequency comb generation and quantum mirrors. The dark state of subradiance, on the other hand, is essential for the quantum memory implementation. Also, nontrivial phenomenons also occur when multiple photons interacting with a single atom simultaneously. When a finite number of photons incidents on an atom, their scattering through an atom is highly nonlinear, and one special eigenstate component of such nonlinear process, namely photonic bound states, exhibits many interesting properties in nonlinear quantum optical systems. The photons in such state are strongly bunched with each other, as if a virtual attractive force is in effect. Also, the frequency of photons are anti-correlated so that their total frequency remains a constant value, no matter how arbitrary the frequency of any individual is. Thesefeatures benefit certain nonlinear quantum processes for quantum computing and quantum imaging. Specially for two-photon excitation imaging, the same-parity two-level fluorophore molecules suffers from extremely low excitation efficiencies due to the far off-resonant intermediate states. However, by replacing the current commonly used ultrashort laser pulse illuminations with two photon bound state photon pairs, namely photonic dimers, the efficiency can be enhanced to orders of magnitude higher. Such exceptionally high excitation efficiency can potentially bring the current in vivo deep brain imaging depth from millimeter level to several centimeters. To obtain a stable source of such photonic dimers, it is found that a laser structure with gain medium of two-photon emission materials is capable of generating the coherent state of photonic dimer and can serve as a promising light source for nonlinear quantum optical devices.