We explore how collective states of light and matter differ when the multi-level nature of the quantum emitters is fully taken into account. For closely spaced emitters, interferences between near-resonant transitions completely change the character of the collective states compared to two-level approximations. In particular, we find a lower bound on the emitter separation for superradiance to occur which does not exist for two-level emitters. By contrast, for larger separations between the emitters, the collective states resemble those obtained within the widely used two-level approximation of the emitters. Both regimes may be realized by molecules trapped in optical lattices. We therefore propose molecular candidates and describe experimental signatures of emerging multi-level interference.
We explore how collective states of light and matter differ when the multi-level nature of the quantum emitters is fully taken into account. For closely spaced emitters, interferences between near-resonant transitions completely change the character of the collective states compared to two-level approximations. In particular, we find a lower bound on the emitter separation for superradiance to occur which does not exist for two-level emitters. By contrast, for larger separations between the emitters, the collective states resemble those obtained within the widely used two-level approximation of the emitters. Both regimes may be realized by molecules trapped in optical lattices. We therefore propose molecular candidates and describe experimental signatures of emerging multi-level interference.
The interaction of light with nanometer-sized structures is at the core of nano-optics. It is obvious that as the particles become smaller and smaller the laws of quantum mechanics will become apparent in their interaction with light. In this limit, continuous scattering and absorption of light will be supplemented or replaced by resonant interactions if the photon energy hits the energy difference of discrete internal (electronic) energy levels. In atoms, molecules and nanoparticles, like semiconductor nanocrystals and other “quantum confined” systems, these resonances are found at optical frequencies. Due to the resonant character, the light–matter interaction can often be approximated by treating the quantum system as an effective two-level system, i.e. by considering only those two (electronic) levels whose difference in energy is close to the interacting photon energy ħ ω 0 . In this chapter we consider single-quantum systems that are fixed in space, either by deposition to a surface or by being embedded into a solid matrix. The material to be covered should familiarize the reader with single-photon emitters and with concepts developed in the field of quantum optics. While various theoretical aspects related to the fields emitted by a quantum system have been discussed in Chapter 8, the current chapter focuses more on the nature of the quantum system itself. We adopt a rather practical perspective since more rigorous accounts can be found elsewhere (see e.g. [1–4]).
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.
We investigate the emergence of cooperative radiation phenomena in ensembles of two-level atoms coupled to a lossy resonant cavity beyond the Markovian and mean-field approximations. By deriving a complete analytical solution for the two-emitter case and employing a numerically exact method for larger ensembles, we characterize the full transition from Markovian to non-Markovian collective dynamics for systems of up to 103 emitters. Our results reveal three distinct regimes: a Markovian phase exhibiting the standard superradiant burst, a non-Markovian phase featuring spontaneous superabsorption of the emitted field, and a critical regime marked by pulsed collective emission. We show that the critical spectral width separating these behaviors increases monotonically with the number of emitters, demonstrating that environmental memory effects can be enhanced by cooperativity. Finally, we find that the superradiant scaling of the peak intensity progressively degrades with increasing system size, approaching a subquadratic law in the limit of a perfect cavity. In this regime, spontaneous superabsorption emerges as a distinct manifestation of non-Markovian cooperativity.
We experimentally investigate the collective radiative decay of a fully inverted ensemble of two-level atoms for a chiral, i.e., propagation direction-dependent light-matter coupling. Despite a fundamentally different interaction Hamiltonian which has a reduced symmetry compared to the standard Dicke case of superradiance, we do observe a superradiant burst of light. The burst occurs above a threshold number of atoms, and its peak power scales faster with the number of atoms than in the case of free-space Dicke superradiance. We measure the first-order coherence of the burst and experimentally distinguish two regimes, one dominated by the coherence induced during the excitation process and the other governed by vacuum fluctuations. Our results shed light on the collective radiative dynamics of cascaded quantum many-body systems, i.e., systems in which each quantum emitter is only driven by light radiated by emitters that are upstream in the cascade. Our findings may turn out useful for generating multiphoton Fock states as a resource for quantum technologies. Published by the American Physical Society 2024
This work focuses on the many-body properties of semiconductor nanostructures for quantum engineering of infrared optoelectronic devices. In particular, we theoretically investigate the optical response accounting for collective effects in systems of tunnel-coupled quantum wells. A clear manifestation of these effects appears in the optical spectrum of highly doped quantum wells, where the absorption peaks are at completely different energies with respect to the single-particle electronic transitions. We calculate light-matter interaction in two steps. First, we consider the microscopic polarization associated with the electronic transitions between confined levels of the wells, which are all coupled by dipole-dipole Coulomb interaction. Then we calculate the interaction of the resulting collective states with the electromagnetic field. The absorption spectrum is finally expressed in terms of microscopic currents, describing the collective charge oscillations. The theoretical model is applied to a series of relevant systems, and its outcomes are compared with experimental results. As the collective states are issued from the coherent superposition of several electronic excitations, they have the properties of superradiant states. They are thus a promising entity for the realization of efficient light emitters in the mid- and far-infrared frequency range.
This thesis contributes to the field of collective effects in atomic ensembles. We explore synchronization of superradiant lasers in different coupling configurations and study superradiance in off-resonantly probed atomic ensembles, where we take into account the complete level structure of alkali metal atoms. In the first part we introduce the superradiant laser and extend the discussion of synchronization of symmetrically coupled superradiant lasers to unidirectional coupled superradiant lasers. We show that synchronization is also present when we replace the superradi- ant laser couplings with classical channels, meaning the synchronization can be considered a classical effect. In the second part we generalize a widely used approximation method taking into account lower order atom-atom correlations — the cumulant expansion method — to a basis independent formalism. We implement this formalism in a Python program allowing us to numerically calculate the n-atom reduced density matrix and two-time correlation functions for ensembles of multi-level atoms. This method allows us to study the stationary state of an ensemble of off-resonantly probed alkali metal atoms with a ground-state manifold consisting of many hyperfine levels. We show that collective effects in light-matter interaction depends on the tensor-polarizability of atoms and therefore cannot be explained on the basis of two-level-approximations.