Abundance of cavity-free polaritonic states in resonant materials and nanostructures

Canales, Adriana; Baranov, Denis G.; Antosiewicz, Tomasz J.; Shegai, Timur

doi:10.1063/5.0033352

Cited by 50 publications

(67 citation statements)

References 69 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Unlike the recent study of strong coupling in self-assembled organic semiconductors by Rao et al, 25 our sample fabrication only uses spin-coating, and our coupling strengths are an order of magnitude greater. Our results suggest that polaritonic effects might be much more prevalent than previously thought, 26 paving the way for simplified strong coupling experiments.…”

mentioning

confidence: 55%

“… 30 The optical constants for our SPI and MC films are given in Figure 1 c; they were determined using spectroscopic ellipsometry (with SPI fitted to a Cauchy dielectric model and MC to a Lorentzian model - see Supplementary Section S1 for fit parameters). The measured optical constants suggest that MC can support bulk polaritons 26 with a Rabi splitting large enough to allow ultrastrong coupling (see Supplementary Section S3 ). The large contrast in permittivity between the SPI/MC films (ϵ SPI = 2.58 at 2.22 eV) and the Si substrate (ϵ Si = 16.3 at 2.22 eV), and between the SPI/MC films and the air superstrate leads to the formation of a series of leaky modes in the film for both transverse electric (TE) and transverse magnetic (TM) polarized light.…”

mentioning

confidence: 91%

“…However, repeating the SPI-MC experiment in Figure 2 , but this time using a glass substrate (in which case the dielectric film has a slightly greater permittivity than the substrate), produces no clear signature of strong coupling (see Supplementary Section S9 ); in this type of structure, fully guided modes and self-hybridization are possible beyond the light-line. 26 , 36 …”

mentioning

confidence: 99%

See 2 more Smart Citations

Cavity-Free Ultrastrong Light-Matter Coupling

Thomas

Menghrajani

Barnes

2021

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

Strong coupling between light and matter can occur when the interaction strength between a confined electromagnetic field and a molecular resonance exceeds the losses to the environment, leading to the formation of hybrid light–matter states known as polaritons. Ultrastrong coupling occurs when the coupling strength becomes comparable to the transition energy of the system. It is widely assumed that the confined electromagnetic fields necessary for strong coupling to organic molecules can only be achieved with external structures such as Fabry–Pérot resonators, plasmonic nanostructures, or dielectric resonators. Here we show experimentally that such structures are unnecessary and that a simple dielectric film of dye molecules supports sufficiently modified vacuum electromagnetic fields to enable room-temperature ultrastrong light-matter coupling. Our results may be of use in the design of experiments to probe polaritonic chemistry and suggest that polaritonic states are perhaps easier to realize than previously thought.

show abstract

mentioning

confidence: 55%

mentioning

confidence: 91%

mentioning

confidence: 99%

See 1 more Smart Citation

Cavity-Free Ultrastrong Light-Matter Coupling

Thomas

Menghrajani

Barnes

2021

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

show abstract

“…highlighted in ref. 35,61,62 . These results show that the maximum coupling strength between a cavity mode and a dipolar excitation is governed by that of photons and bulk, implying that fully filling a resonant cavity with a specific material does not enhance the coupling strength between light and matter.…”

Section: Discussionmentioning

confidence: 99%

Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime

et al. 2021

View full text Add to dashboard Cite

Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ultrastrong coupling in fully filled cavities yields a polariton dispersion matching that of phonon polaritons in bulk hBN, highlighting that the maximum light-matter coupling in microcavities is limited to the coupling strength between photons and the bulk material. Tunable cavity phonon polaritons could become a versatile platform for studying how the coupling strength between photons and phonons may modify the properties of polar crystals.

show abstract

“…9 Even more so, they are suitable for obtaining self-hybridized polaritons, for potentially changing the material properties of a sample. 10,11 These resonances are particularly relevant in the field of optical trapping. In fact, Arthur Ashkin observed Mie resonances in the scattering force of an optically levitated solid micro-particle.…”

Section: Mainmentioning

confidence: 99%

Revealing Fano Combs in Directional Mie Scattering

Marmolejo

Canales

Hanstorp

et al. 2021

Preprint

Self Cite

View full text Add to dashboard Cite

The constructive interference of light reflecting on the inner surface of a dielectric sphere results in a rich Mie scattering spectrum. Each resonance can be understood through a quantum-mechanical analogy, while the structure of the full spectrum is predicted to be a series of Fano resonances. However, the overlap of all the different modes results in such a complex spectrum that an intuitive understanding of the full, underlying structure is still missing. Here we present a directional Mie spectrum obtained by selecting a particular polarization and direction of the scattering of levitating water droplets. We find a significantly simplified spectrum organized in distinct, consecutive Mie Fano Combs composed of equidistant resonances that smoothly evolve from wide Lorentzians into sharp Fano profiles. We then fully explain all these characteristics by expanding on the quantum-mechanical analogy. This makes it possible to understand Mie spectra intuitively without the need for computational simulations.

show abstract

Abundance of cavity-free polaritonic states in resonant materials and nanostructures

Abstract: Note: This paper is part of the JCP Special Topic on Polariton Chemistry: Molecules in Cavities and Plasmonic Media.

Cited by 50 publications

References 69 publications

Cavity-Free Ultrastrong Light-Matter Coupling

Cavity-Free Ultrastrong Light-Matter Coupling

Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime

Revealing Fano Combs in Directional Mie Scattering

Contact Info

Product

Resources

About