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Proceedings of the National Academy of Sciences

Hybridization of molecules via a common photonic mode

Jahangir Nobakht, André Pscherer, Jan Renger, Stephan Götzinger, Vahid Sandoghdar

Published Jul 30, 2025• 5 citations
Publisher

Abstract

Atoms and molecules usually hybridize and form bonds when they come in very close proximity of each other. In this work, we show that molecules can hybridize even through far-field electromagnetic interactions mediated by the shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and subradiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.

DOI
10.1073/pnas.2505161122

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Atoms and molecules usually hybridize and form bonds when they come in very close proximity of each other. In this work, we show that molecules can hybridize even through far-field electromagnetic interactions mediated by the shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and subradiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.
Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.
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'.
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.
Optical microcavities and metallic nanostructures have been shown to significantly modulate the dynamics and spectroscopic response of molecular systems. We present a study of the nonlinear optics of a model consisting of NNN anharmonic multilevel systems (e.g., Morse oscillators) undergoing collective strong coupling with a resonant infrared microcavity. We find that, under experimentally accessible conditions, molecular systems in microcavities may have nonlinear phenomena significantly intensified due to the high quality of polariton resonances and the enhanced microcavity electromagnetic energy density relative to free space. Particularly large enhancement of multiphoton absorption happens when multipolariton states are resonant with bare molecule multiphoton transitions. In particular, our model predicts two-photon absorption cross-section enhancements by several orders of magnitude relative to free space when the Rabi splitting ${\mathrm{\ensuremath{\Omega}}}_{R}$ is approximately equal to the molecular anharmonic shift $2\mathrm{\ensuremath{\Delta}}$. Our results provide rough upper bounds to resonant nonlinear-response enhancement factors as relaxation to dark states is treated phenomenologically. Notably, ensembles of two-level systems undergoing strong coupling with a cavity (described by the Tavis-Cummings model) show no such optical nonlinearity enhancements, highlighting the rich phenomenology afforded by multilevel anharmonic systems. Similar conclusions are expected to hold for excitonic systems that share features with our model (e.g., molecular dyes with accessible ${S}_{0}\ensuremath{\rightarrow}{S}_{1}\ensuremath{\rightarrow}{S}_{2}$ transitions) and strongly interact with a UV-visible cavity.
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.
We demonstrate photon-mediated interactions between two individually trapped atoms coupled to a nanophotonic cavity. Specifically, we observe collective enhancement when the atoms are resonant with the cavity and level repulsion when the cavity is coupled to the atoms in the dispersive regime. Our approach makes use of individual control over the internal states of the atoms and their position with respect to the cavity mode, as well as the light shifts to tune atomic transitions individually, allowing us to directly observe the anticrossing of the bright and dark two-atom states. These observations open the door for realizing quantum networks and studying quantum many-body physics based on atom arrays coupled to nanophotonic devices.