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arXiv:2605.01583

Strong light-matter interactions in hybrid polaritonic systems

Ben Johns, Andrea Schirato, Federico Toffoletti, Tommaso Giovannini, Mirko Vanzan, Margherita Marsili, Giovanni Parolin, Giulia Dall'Osto, Ajay Kumar Poonia, Chiara Cappelli, Francesca Baletto, Stefano Corni, Elisabetta Collini, Margherita Maiuri, Nicolò Maccaferri

physics.opticscond-mat.mtrl-sciphysics.chem-phquant-phSubmitted May 2, 2026• Announced May 5, 2026
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Abstract

Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.

AI Summary

This Feature Article surveys how strong light–matter coupling produces polaritons and how their mixed photonic and material character can affect optical, electronic, and chemical behavior. Its scope spans the physical platforms used to achieve coupling, the materials involved, and the mechanisms connecting polariton formation to transport and reactivity. The article covers photonic microcavities, plasmonic nanostructures, open cavities, and metasurfaces, alongside inorganic semiconductors, organic aggregates, and hybrid material systems. It outlines access to strong- and ultrastrong-coupling regimes and discusses coherent dynamics, vibronic interactions, dark-state reservoirs, and polariton-mediated energy and electron transport. It also surveys experimental and theoretical tools used to investigate these effects. Examples are described in which strong coupling modifies charge transport, energy flow, or chemical reactivity, while intermediate and dark-strong coupling are presented as emerging regimes extending the range of hybrid light–matter phenomena. The abstract presents this as a survey rather than a report of a new experiment, calculation, or quantitative bound. It provides no coupling strengths, transport enhancements, reaction-rate changes, or other numerical benchmarks, and does not specify the evidence supporting individual examples or how competing interpretations are assessed. No explicit limitations are stated in the abstract. Because the full text is unavailable, the depth of coverage, criteria distinguishing the coupling regimes, and treatment of unresolved experimental and theoretical questions cannot be determined.

No sign of AI-generated text

Written by gpt-6.1-sol from the abstract only. Automated: it can be wrong.

DOI
10.1039/D6CC02672A

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Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.
This Feature Article surveys how strong light–matter coupling produces polaritons and how their mixed photonic and material character can affect optical, electronic, and chemical behavior. Its scope spans the physical platforms used to achieve coupling, the materials involved, and the mechanisms connecting polariton formation to transport and reactivity.
The article covers photonic microcavities, plasmonic nanostructures, open cavities, and metasurfaces, alongside inorganic semiconductors, organic aggregates, and hybrid material systems. It outlines access to strong- and ultrastrong-coupling regimes and discusses coherent dynamics, vibronic interactions, dark-state reservoirs, and polariton-mediated energy and electron transport. It also surveys experimental and theoretical tools used to investigate these effects. Examples are described in which strong coupling modifies charge transport, energy flow, or chemical reactivity, while intermediate and dark-strong coupling are presented as emerging regimes extending the range of hybrid light–matter phenomena.
The abstract presents this as a survey rather than a report of a new experiment, calculation, or quantitative bound. It provides no coupling strengths, transport enhancements, reaction-rate changes, or other numerical benchmarks, and does not specify the evidence supporting individual examples or how competing interpretations are assessed. No explicit limitations are stated in the abstract. Because the full text is unavailable, the depth of coverage, criteria distinguishing the coupling regimes, and treatment of unresolved experimental and theoretical questions cannot be determined.
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the high energy shift of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that affect nonlinear dynamics and change mechanisms of polariton energy shifts accordingly. We have scrutinized the origins of energy shifts in connection with nonlinear dynamics in Frenkel exciton-polariton condensates and examined the possible contributions: intracavity optical Kerr-effect, gain-induced frequency pulling, polariton interactions and effects related to saturation of optical transitions for "dark"- and "bright" molecules [1]. Unlike the conventional strongly coupled semiconductor microcavities, we have shown that nonlinear interactions within the condensate do not rely on polariton interactions but instead originated from Pauli-blocking principle forbidding double excitation of the same molecular states. We have developed a theoretical model explaining the omnipresent energy shift of the condensate wavefunction together with its spectral and polarization features at the BEC transition in a consistent way. The crucial role of intermolecular energy transfer and “dark” exciton reservoir has been demonstrated for the first time. We believe the principles explored in this work are relevant to other systems exhibiting strong coupling of Frenkel excitons with a cavity mode, regardless of a cavity type, whether one dealing with Fabry-Perot cavities or plasmonic nanocavities etc and; therefore, provide general insight on nonlinear phenomena in composite light-matter condensates. [1] T. Yagafarov, D. Sannikov, A. Zasedatelev, K. Georgiou, A. Baranikov, O. Kyriienko, I. Shelykh, L. Gai, Z. Shen, D. G. Lidzey, P. Lagoudakis, Mechanisms of blueshifts in organic polariton condensates, Commun Phys 3, 18 (2020). https://doi.org/10.1038/s42005-019-0278-6
Ultrastrong coupling between light and matter has, in the past decade, transitioned from a theoretical idea to an experimental reality. It is a new regime of quantum light–matter interaction, which goes beyond weak and strong coupling to make the coupling strength comparable to the transition frequencies in the system. The achievement of weak and strong coupling has led to increased control of quantum systems and to applications such as lasers, quantum sensing, and quantum information processing. Here we review the theory of quantum systems with ultrastrong coupling, discussing entangled ground states with virtual excitations, new avenues for nonlinear optics, and connections to several important physical models. We also overview the multitude of experimental setups, including superconducting circuits, organic molecules, semiconductor polaritons, and optomechanical systems, that have now achieved ultrastrong coupling. We conclude by discussing the many potential applications that these achievements enable in physics and chemistry.
Attempting to implement quantum information related applications utilizing atoms and photons, as they naturally form quantum systems supporting superposition states, hybrid quantum plasmonic systems emerged in the past as a platform to study and engineer light-matter interaction. This platform combines the unrivaled electromagnetic field localization of surface plasmon polaritons, boosting the light-matter coupling rate, with the tremendous integration potential of truly nanoscale structures, and both the significant emission rates of nanoantennas and photonic transmission velocities. In this work, a classical description of surface plasmon polaritons is combined with a light-matter interaction model based on a cavity quantum electrodynamical formalism. The resulting composite semi-classical method, introduced and described in this thesis, provides efficient and versatile means to simulate the dynamical behavior of radiative atomic transitions coupled to plasmonic cavity modes in the weak incoherent coupling regime. Both the emission into the far field and various dissipation mechanisms are included by expanding the model to an open quantum system. The variety of light-matter interaction applications that can be modeled with the outlined method is indicated by the four different exemplary scenarios detailed in the application chapter of this thesis. The classical description of localized surface plasmon polaritons is benchmarked by reproducing the experimental measurements of the molecular fluorescence manipulation through optical nanoantennas in a collaborative effort with experimental partners. Furthermore, in the weak light-matter coupling regime, the potential of achieving a higher nanoantenna functionality and simultaneously realizing more elaborate quantum dynamics is revealed by the three remaining applications. Each pivotally involving a bimodal nanoantenna and demonstrating different quantum optical phenomena, the implementation of cavity radiation mode conversion, non-classical cavity emission statistics, and non-classical cavity emission properties is shown and described in the application chapter.
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET) dynamics in cavity-coupled molecules using the numerically exact hierarchical equations of motion (HEOM) method, which captures nonperturbative and non-Markovian effects beyond standard perturbative theories. We identify distinct resonance and collective effects associated with polariton formation and show that the ET rate saturates in the strong-coupling regime, a feature not captured by perturbative approaches. We further extend the cavity-modified ET model by incorporating the nuclear-coordinate dependence of molecular electric dipole moments, which gives rise to a three-body interaction involving molecular electronic and vibrational degrees of freedom and cavity photons. This vibronic polariton formation leads to non-monotonic, oscillatory dependencies of the ET rate on the light-matter coupling strength and cavity frequency, which we attribute to quantum interference among multiple transfer pathways. These findings establish cavity-modified electron transfer as a multichannel quantum process governed by the interplay of electronic, vibrational, and photonic degrees of freedom.
This dissertation studies the effects of strong matter-light coupling on properties of organic molecules and inorganic semiconductors. The interplay of complex intramolecular dynamics and strong coupling of a photon to molecular transitions results in new physics having no counterparts in other systems. In contrast, low-energy optically active excitations of semiconductors (excitons) usually do not feature such complexity. However, the combination of strong electronic correlations and strong matter-light coupling leads to new physics. Firstly, the effect of strong coupling between molecular vibrations and infrared photons on Raman scattering (RS) is considered. This is motivated by the experiment of Ref. [1] showing up to 10³ enhancement of RS signal under strong coupling. While the exact analytical results of this dissertation predict around 100% enhancement of total RS signal, they cannot explain orders of magnitude enhancement, leaving the question open for further studies. Next, the effects of strong coupling of an optical photon and a molecular electronic transition on molecular lasing properties are discussed. Starting from a microscopic description of a driven-dissipative system, an exact (in the thermodynamic limit) mean-field solution is developed. It allows to uncover the mechanism of molecular lasing in the weak and strong coupling regime and to obtain a non-equilibrium lasing phase diagram. Finally, a semiconductor with different densities of electrons and holes, strongly coupled to a microcavity photon, is studied. While finite electron-hole density imbalance is detrimental for excitonic condensation, it may still lead to a condensed state of excitons with finite centre of mass momentum coexisting with unpaired electrons. On the other hand, due to its low mass, a photon favours zero center of mass momentum condensation. The variational mean-field calculations reveal that the interplay of these effects leads to a variety of novel states with coexisting polariton condensate and unpaired electrons.
We demonstrate that a ionising transition can be strongly coupled to a photonic resonator, leading to the appearance of a discrete optically active polaritonic resonance below the ionisation threshold. The matter component of such hybrid excitation corresponds to a bound exciton created by light-matter interaction. Applying our theory to the case of bound-to-continuum transitions in microcavity-embedded doped quantum wells, we show how those strong-coupling features can be exploited as a novel gauge to tune both optical and electronic properties of semiconductor heterostructures.