Tuning materials' properties by non-perturbative cavity quantum electrodynamics

Abstract

When in a quantum optical system the coupling between matter and cavity mode becomes comparable to the bare excitation frequency, we enter a non-perturbative coupling regime, as perturbation theory fails describing the system’s dynamics. While recent advances in Cavity Quantum Electrodynamics allowed to achieve very high values of the coupling strength, thanks to the resonators properties optimization and the employment of solid-state devices, an ever growing interest has been shown about the possibility of significantly modify materials’ properties. It has been demonstrated that the chemical structure of molecules strongly coupled to a photon mode can be altered, which opens the possibility to manipulate and control chemical reactions.

The aim of this thesis is to explore non-perturbative regimes on several quantum systems, and to investigate the effects of the coupling upon their properties, such as internal degrees of freedom or electronic states structure. I first developed a novel theory to determine the polariton spectrum of a dipolar ensamble in which a Ising-like dipole-dipole interaction in the 2 non-perturbative regime is considered. A further important focus is the investigation of the saturation effects due to the inclusion of the inter-dipole interaction, and the interplay between the latter and light-matter coupling strength. I also explored specifically the influence of the coupling on the rotational degrees of freedom of an ensemble of two-dimensional freely rotating dipoles, all coupled to a single cavity mode, finding that they are driven by the collective light-matter coupling to undergo a crossover between an isotropic and an aligned phase. I then investigated the case of cavity-embedded doped quantum wells, demonstrating that not only it is possible to couple a discrete cavity mode and bound-to-continuum transitions, but also that a novel bound exciton state appears, induced by the coupling strength. This results shows how light–matter coupling can be used to tune both optical and electronic properties of semiconductor heterostructures beyond those permitted by mere crystal properties. Finally, I explored the physics of an array of THz metamaterial resonators coupled to cyclotron resonances of a two-dimensional electron gas, developing a multiple-mode theory that takes in account the interaction between multiple photon modes mediated by the electrons. My results show that this cross-interaction, due to the strong two-dimensional geometry of the optically active medium, leads to the hybridization of different uncoupled photon modes, and manifests as a visible change of the distribution of the coupled electromagnetic field.

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Identifiers

ORCID for Simone De Liberato: orcid.org/0000-0002-4851-2633

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