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arXiv:2311.00183 · Physical review. B./Physical review. B

Electrostatic nature of cavity-mediated interactions between low-energy matter excitations

Petros Andreas Pantazopoulos, Johannes Feist, Akashdeep Kamra, Francisco José García-Vidal

Published May 23, 2024• 5 citations
arXivHTMLPDF

Abstract

Here, the authors demonstrate that cavity quantum electrodynamical effects induce electrostatic interactions between low-energy matter excitations when these are off-resonantly coupled either directly to the cavity field or indirectly via resonant mediator modes. These findings expose the limitations of previous models that have used just one cavity mode in the electromagnetic description of the cavity. The results provide critical insights for designing nanophotonic structures leading to significant cavity-induced interactions, which could open new avenues for modifying material properties using vacuum fields.

DOI
10.1103/physrevb.109.l201408

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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'.
We address the fundamental question of whether or not it is possible to achieve conditions under which the coupling of a single dipole to a strongly confined electromagnetic vacuum can result in nonperturbative corrections to the dipole's ground state. To do so we consider two simplified, but otherwise rather generic cavity QED setups, which allow us to derive analytic expressions for the total ground-state energy and to distinguish explicitly between purely electrostatic and genuine vacuum-induced contributions. Importantly, this derivation takes the full electromagnetic spectrum into account while avoiding any ambiguities arising from an ad hoc mode truncation. Our findings show that while the effect of confinement per se is not enough to result in substantial vacuum-induced corrections, the presence of high-impedance modes, such as plasmons or engineered LC resonances, can drastically increase these effects. Therefore, we conclude that with appropriately designed experiments it is at least in principle possible to access a regime where light-matter interactions become nonperturbative.
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Confining electromagnetic fields inside an optical cavity can enhance the light–matter coupling between quantum materials embedded inside the cavity and the confined photon fields. When the interaction between the matter and the photon fields is strong enough, even the quantum vacuum field fluctuations of the photons confined in the cavity can alter the properties of the cavity-embedded solid-state materials at equilibrium and room temperature. This approach to engineering materials with light avoids fundamental issues of laser-induced transient matter states. To clearly differentiate this field from phenomena in driven systems, we call this emerging field cavity materials engineering . In this review, we first present theoretical frameworks, in particular, ab initio methods, for describing light–matter interactions in solid-state materials embedded inside a realistic optical cavity. Next, we overview a few experimental breakthroughs in this domain, detailing how the ground state properties of materials can be altered within such confined photonic environments. Moreover, we discuss state-of-the-art theoretical proposals for tailoring material properties within cavities. Finally, we outline the key challenges and promising avenues for future research in this exciting field.