Mie excitons: Understanding strong coupling in dielectric nanoparticles

Tserkezis, Christos; Gonçalves, P. A. D.; Wolff, Christian; Todisco, Francesco; Busch, Kurt; Mortensen, N. Asger

doi:10.1103/physrevb.98.155439

Cited by 48 publications

(51 citation statements)

References 80 publications

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“…This shows that the scattering observed for the coupled cavity does not result from surface roughness of the cavity mirrors or some enhancement of scattering due to multiple reflections at the cavity resonance. We note that the lack of scattering from the empty cavity indicates that the observed scattering in the coupled system is fundamentally different than the scattering reported for hybrid moleculenanoparticle systems [39][40][41], in which the optical resonator has a high scattering cross section by itself, even without the molecules. Moreover, AFM measurements of the cavities (Figs.…”

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confidence: 65%

Collective Rayleigh Scattering from Molecular Ensembles under Strong Coupling

Golombek

Balasubrahmaniyam

Kaeek

et al. 2020

J. Phys. Chem. Lett.

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Rayleigh scattering is usually considered to be the elastic scattering of photons from subwavelength physical objects, such as small particles or molecules. Here, we present the spectroscopic study of the scattering properties of molecules embedded in an optical cavity under strong coupling conditions, where the collective interaction between the molecules and the cavity gives rise to composite light-matter excitations known as cavity polaritons. We show that the polaritonic states exhibit strong resonant Rayleigh scattering, reaching ∼ 25% efficiency. Since the polaritonic wavefunctions in such systems are delocalized, our observations correspond to the collective scattering of each photon from a large ensemble of molecules.When quantum emitters are placed inside an optical cavity, their interaction with the quantized electromagnetic mode of the cavity may become large enough to overcome the incoherent processes taking place in the system [1]. This regime, which is known as strong light-matter coupling, has been extensively studied in hybrid molecular-photonic systems over the past decade, as it offers exciting possibilities for controlling the photophysical and chemical properties of molecules [2,3]. The coupling between an ensemble of molecules and an optical resonator is quantified by the vacuum Rabi frequency, which is roughly given byHere d is the transition dipole element of the molecules, is Planck's constant, ω c is the cavity resonance frequency, is the background dielectric constant inside the cavity, V c the cavity mode volume and N is the number of molecules inside the cavity. The √ N dependence of the coupling strength indicates that, under strong coupling conditions, the interaction between the molecules and the optical mode is collective. As a result, the eigenstates of the coupled system, known as cavity polaritons, represent a coherent superposition of a photon and a material excitation which is delocalized across a macroscopically large ensemble of molecules [1,4]. The collective nature of strong coupling in molecular systems is currently attracting considerable attention [5][6][7][8][9][10], as it gives rise to fascinating effects. These include, for instance, long-range spatial coherence [11][12][13], enhanced transport [14-18] and energy transfer [19][20][21], and even collective molecular reactivity [22][23][24][25].The progress in this evolving field is intimately linked to the extensive spectroscopic study of organic strongly coupled systems, which has gradually revealed the properties of the polari- * Corresponding author talschwartz@tau.ac.il

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confidence: 65%

Collective Rayleigh Scattering from Molecular Ensembles under Strong Coupling

Golombek

Balasubrahmaniyam

Kaeek

et al. 2020

J. Phys. Chem. Lett.

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“…In this review, we shall consider that the “emitter” is represented by an excitonic resonance ascribed to the 2D TMDC (Figure b); in such a case, the previous expression cannot be employed directly and an explicit formula for the coupling energy is in general a nontrivial and onerous task (for a discussion about this predicament, see, for instance, ref. and references therein). Notwithstanding, one may still in principle define an effective coupling ( g  g eff herein) that could be inferred from experimental data.…”

Section: Strong Light–matter Interactions In Layered Transition Metalmentioning

confidence: 99%

Strong Light–Matter Interactions Enabled by Polaritons in Atomically Thin Materials

Gonçalves

Stenger

Cox

et al. 2020

Advanced Optical Materials

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Polaritons, resulting from the hybridization of light with polarization charges formed at the boundaries between media with positive and negative dielectric response functions, can focus light into regions much smaller than its associated free‐space wavelength. This property is paramount for a plethora of applications in nanophotonics, ranging from biological sensing to photocatalysis to nonlinear and quantum optics. In the two‐dimensional (2D) limit, represented by atomically thin and van der Waals (vdW) materials of single‐layers bound by weak vdW attraction, polaritons are characterized by extremely small wavelengths associated with extreme optical confinement, and furthermore can exhibit long lifetimes, electrical tunability, and extreme sensitivity to their dielectric environment, among many other desirable qualities in nano‐optical device applications. Here, the fundamentals of polaritons in atomically thin materials are summarized, emphasizing plasmon and exciton polaritons, their strong light–matter interactions, and nonlinear plasmonics. More specifically, this review opens with a pedagogical discussion of plasmons in extended and nanostructured graphene, providing a classical electrodynamical model in a nonretarded theoretical framework, and the ultraconfined acoustic plasmons supported by hybrid graphene–dielectric–metal structures. In addition, the basic principles are introduced and the recent developments on nonlinear graphene plasmonics and on strong coupling physics with atomically thin transition metal dichalcogenides are reviewed. Finally, potentially new, promising research directions in the burgeoning field of 2D nanophotonics are identified.

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“…Molecular strong coupling with Mie resonances in dielectric nanoparticles have been demonstrated theoretically 32,33 and experimentally. 34,35 On the other hand WGM based cavities like microdiscs and toroids have been utilized to strongly couple atoms, 36 ions, 37 and quantum dots 38,39 at cryogenic temperatures.…”

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Molecular Monolayer Strong Coupling in Dielectric Soft Microcavities

Vasista

Barnes

2020

Nano Lett.

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We report strong coupling of a monolayer of J -aggregated dye molecules to the whispering gallery modes of a dielectric microsphere at room temperature. We systematically studied the evolution of strong coupling as the number of layers of dye molecules was increased, we found the Rabi splitting to rise from 56 meV for a single layer to 94 meV for four layers of dye molecules. We compare our experimental results with 2D numerical simulations and a simple coupled oscillator model, finding good agreement.We anticipate that these results will act as a stepping stone for integrating moleculecavity strong coupling in a microfluidic environment since microspheres can be easily trapped and manipulated in such an environment, and provide open access cavities.

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Mie excitons: Understanding strong coupling in dielectric nanoparticles

Cited by 48 publications

References 80 publications

Collective Rayleigh Scattering from Molecular Ensembles under Strong Coupling

Collective Rayleigh Scattering from Molecular Ensembles under Strong Coupling

Strong Light–Matter Interactions Enabled by Polaritons in Atomically Thin Materials

Molecular Monolayer Strong Coupling in Dielectric Soft Microcavities

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