Optical cavity/molecule strong coupling offers attractive opportunities to modulate photochemical or photophysical processes. When atoms or molecules are placed in an optical cavity, they can coherently exchange photonic energy with optical cavity vacuum fields, entering the strong coupling interaction regime. Recent work suggests that the thermodynamic and kinetic properties of molecules can be significantly changed by strong coupling, resulting in the emergence of intriguing photochemical and photophysical phenomena. As more and more physico-chemical systems are studied under strong coupling conditions, optical cavities have also advanced in their sophistication, responsiveness, and (multi)functionality. In this review, we highlight some of these recent developments, particularly focusing on Fabry-Perot microcavities.
Optical cavity/molecule strong coupling offers attractive opportunities to modulate photochemical or photophysical processes. When atoms or molecules are placed in an optical cavity, they can coherently exchange photonic energy with optical cavity vacuum fields, entering the strong coupling interaction regime. Recent work suggests that the thermodynamic and kinetic properties of molecules can be significantly changed by strong coupling, resulting in the emergence of intriguing photochemical and photophysical phenomena. As more and more physico-chemical systems are studied under strong coupling conditions, optical cavities have also advanced in their sophistication, responsiveness, and (multi)functionality. In this review, we highlight some of these recent developments, particularly focusing on Fabry-Perot microcavities.
Abstract Control of light–matter coupling at the quantum level is an enabling technique for many emerging quantum technologies. This tutorial describes recent advances in achieving efficient coupling of light with a single molecule using an optical Fabry–Perot microcavity. We demonstrate that the efficient cavity-molecule coupling converts the molecule to an effective two-level system. In this regime, a single molecule can act as a nearly perfect reflecting mirror and exhibits optical nonlinearity at the ultimate level of single photons.
Room temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show the that the emergence of a vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low finesse multi-mode situations we find that molecular dipoles can be partially hybridised with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.
Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.
Abstract When atoms come together and bond, these new states are called molecules and their properties determine many aspects of our daily life. Strangely enough, it is conceivable for light and molecules to bond, creating new hybrid light–matter states with far‐reaching consequences for these strongly coupled materials. Even stranger, there is no “real” light needed to obtain the effects; it simply appears from the vacuum, creating “something from nothing.” Surprisingly, the setup required to create these materials has become moderately straightforward. In its simplest form, one only needs to put a strongly absorbing material at the appropriate place between two mirrors, and quantum magic can appear. Only recently has it been discovered that strong coupling can affect a host of significant effects at a material and molecular level, which were thought to be independent of the “light” environment: phase transitions, conductivity, chemical reactions, etc. This review addresses the fundamentals of this opportunity: the quantum mechanical foundations, the relevant plasmonic and photonic structures, and a description of the various applications, connecting material chemistry with quantum information, entanglement, nonlinear optics, and chemical reactivity. Ultimately, revealing the interplay between light and matter in this new regime opens attractive avenues for various new technologies.
The interaction of light with matter is at the heart of quantum optics, which itself enables insight into the fundamental aspects of quantum mechanics. First experimental access to this research field has been realized by coupling atoms to light. Here, the transition between discrete energy states of the atom is associated with the absorption and emission of a photon, a single quantum of the electromagnetic field. As a central aspect of quantum optics, the light-emitter interaction can be significantly enhanced by placing the emitter in optical cavity that is on resonance with the emitter. In recent years, this has led to a rapidly evolving research field known as cavity quantum electrodynamics (CQED). In CQED two different regimes are distinguished: the strong and the weak coupling regimes. In the strong coupling regime, the emitted photon is reflected from the cavity mirrors and eventually reabsorbed by the emitter. In contrast, the weak coupling regime describes the irreversible emission, where the photon leaks out of the cavity before it can be reabsorbed. Both the weak and strong coupling regimes enabled fundamental experiments for a better understanding of quantum optical phenomena. \n \n \n \nCQED grants access to the quantum world and hence offers potentially revolutionizing applications, particularly in the field of quantum information processing. A central aspect for the successful implementation of quantum applications is the system's scalability. Unfortunately, placing atoms deterministically inside a cavity remains technologically elaborate and hence minimizes the prospect of scaling a atom-CQED system. \n \nA possibility to address this issue is to implement CQED in the solid state, where sophisticated fabrication strategies allow miniaturization and scalability of the system. Particularly the development of self-assembled quantum dots (QD) in semiconductors represent a promising route. QDs can be considered as artificial atoms that mimic the atomic two-level system. These structures interact strongly with light and therefore have the potential for replacing atoms in CQED. As a central advantage, QDs are naturally trapped, which greatly simplifies the deterministic incorporation into the cavity. \n \nIn recent years, many efforts have been made to couple self-assembled QDs to microcavities. Generally, the successful implementation of CQED requires a cavity with a high quality factor Q and a low mode volume. In a majority of the approaches, the high Q/small mode volume cavities were monolithically defined around the QD, embedding the QD at a fixed position inside the cavity. Both the weak and strong coupling regimes have been reached with these systems. However, for future applications they suffer from several disadvantages. The fixed position of the QD inside the cavity minimizes the prospects for spectral tunability and spatial positioning the QD inside the cavity. Furthermore, prospects for further increasing of the cavity Q-factor and minimization of the mode volume remain limited in these systems. \n \nIn this thesis the mentioned disadvantages are addressed by developing a fully tunable miniaturized Fabry-Pérot microcavity with low mode volume. The design enables both spatial positioning of the emitter inside the cavity and spectral tunability. Successful coupling of a single QD to the microcavity is demonstrated including the strong coupling regime. Further a new approach to decrease the cavity mode volume is presented, where we demonstrate weak coupling is achieved
The interaction between light and matter has attracted much attention not only for fundamental research but also for applications. The open Fabry-Perot cavity provides an excellent platform for such a study due to strong optical confinement, spectral and spatial and tunability, and the feasibility of optical fiber integration. In this review, first, the basic properties of open Fabry-Perot cavities and the fabrication techniques are introduced. Then recent progress of weak coupling, strong coupling and bad emitter regimes is discussed. Finally, the challenges to and perspectives in this respect are presented.