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Magnetic and electric dipole near-field profiles. Logarithm of total electric field intensity (color scale) and orientation of the real in-plane part of the electric field (arrows) at resonance and under normal incidence, calculated for silicon nanodisks with (A) 150 nm and (B) 230 nm diameter. Here z<0 represents the sapphire substrate. The smaller disk clearly exhibits a magnetic-dipole-like behavior, with a loop in the electric field amplitude inside the particle, while the larger disk shows an electric dipole behavior, with an antinode at the nanodisk center.
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Light-matter interactions at the nanoscale constitute a fundamental ingredient for engineering applications in nanophotonics and quantum optics. In this regard, Mie resonances supported by high-refractive index dielectric nanoparticles have recently attracted interest, due to their lower losses and better control over the scattering patterns compar...
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Citations
... If a shell is formed with a material of very large transition dipole moment, such as J-aggregates, 42 and transition metal dichalcogenides (TMDCs), 44 interaction between a Mie mode and the excitonic state can be in the strong coupling regime. 44,[93][94][95] In 2016, Wang et al. studied resonance coupling between a Mie mode of a Si nanoparticle and the excitonic state of J-aggregate. Figure 6(a) shows the calculated scattering spectra of a Si NP-core/J-aggregate [cyanine dye (TDBC)]-shell (2 nm in thickness) structure 42 assuming a classical Lorentz model for the permittivity of J-aggregate, ...
A silicon nanoparticle with a diameter of 100–300 nm possesses electric- and magnetic-type Mie resonances in the visible to near-infrared ranges and is recognized as a novel nanoplatform that can be used for light propagation control, light–matter interaction enhancement, structural coloration, bio-imaging and -sensing, etc. The functions of a silicon nanoparticle can be greatly extended by decorating the surface with various passive and active materials. In this mini-review, we introduce a recent development of a core/shell architecture made from Mie resonant silicon nanoparticles. We start from the state-of-the-art of the production of high-quality silicon nanoparticles. We then introduce fabrication processes of the core/shell architectures for a variety of shell materials that modify the properties of silicon nanoparticles and introduce new functions. The shell materials include passive low-refractive index materials, materials of tunable optical properties, fluorescence dyes, transition metal dichalcogenides, and noble metals with surface plasmon resonances. Finally, we will discuss our perspective for the development of future silicon-based core/shell architectures.
... These cavities exhibit high-quality optical resonances, known as Mie Surface Lattice Resonances (M-SLRs), resulting from the interaction between the localized Mie resonances of the individual nanoparticles and the in-plane diffraction orders (DOs) of the array. 30,31,32,33,34,35 The M-SLRs concentrate the electromagnetic fields near the array surface. Consequently, when an equilibrated solution of supramolecular TPE assemblies is drop casted onto the nanocavity surface ( Figure S13), 36 the strong fields enhance the interaction of (the excitons in the) TPE fibers with light, resulting in enhanced emission at the resonant wavelengths of the cavity. ...
H-type supramolecular polymers with preferred helicity and highly efficient emission have been prepared from the self-assembly of chiral tetraphenylene-based monomers. Implementation of the one-dimensional fibers into dielectric nanoparticle arrays allows...
... Similarly, spins in microwave cavities produce magnons [32], the collective excitation of electrons in different subbands leads to intersubband polaritons [33], and Landaulevel transitions in 2D electron gases can couple to electric resonators and, under the influence of a strong magnetic field, produce Landau polaritons [34]. More complex polaritons involving the coupling of two quasiparticles (one of the two usually being an exciton) include plexcitons in noble metal nanoparticles (NPs) covered with an excitonic layer [35], perovskite-exciton polaritons [36], and Mie-excitons in high-index dielectric NPs [37], [38], possibly with a magnetooptical character [39]. ...
... For the calculation of the spectra, traditional Mie theory is obviously no longer applicable; we thus employ the nearest equivalent, namely the extended boundary condition method (EBCM) [67], which is still based on spherical-wave expansions. The simulation set-up and all convergence parameters are as described in Ref. [38]. We should note here that, within EBCM, the characterisation of modes in terms of multipoles is straightforward, because the matrix that connects the scattered to the incident field, though not diagonal, is almost always dominated by a single element with specific angular-momentum indices and m; alternatively, one can use Cartesian multipoles [68]. ...
We discuss the possibility of self-hybridisation in high-index dielectric nanoparticles, where Mie modes of electric or magnetic type can couple to the interband transitions of the material, leading to spectral anticrossings. Starting with an idealised system described by moderately high constant permittivity with a narrow Lorentzian, in which self-hybridisation is visible for both plane-wave and electron-beam excitation, we embark on a quest for realistic systems where this effect should be visible. We explore a variety of spherical particles made of traditional semiconductors such as Si, GaAs, and GaP. With the effect hardly discernible, we identify two major causes hindering observation of self-hybridisation: the very broad spectral fingerprints of interband transitions in most candidate materials, and the significant overlap between electric and magnetic Mie modes in nanospheres. We thus depart from the spherical shape, and show that interband–Mie hybridisation is indeed feasible in the example of GaAs cylinders, even with a simple plane-wave source. This so-far unreported kind of polariton has to be considered when interpreting experimental spectra of Mie-resonant nanoparticles and assigning modal characters to specific features. On the other hand, it has the potential to be useful for the characterisation of the optical properties of dielectric materials, through control of the hybridisation strength via nanoparticle size and shape, and for applications that exploit Mie resonances in metamaterials, highly-directional antennas, or photovoltaics.
... Similarly, spins in microwave cavities produce magnons [32], the collective excitation of electrons in different subbands leads to intersubband polaritons [33], and Landau-level transitions in 2D electron gases can couple to electric resonators and, under the influence of a strong magnetic field, produce Landau polaritons [34]. More complex polaritons involving the coupling of two quasiparticles (one of the two usually being an exciton) include plexcitons in noble metal nanoparticles (NPs) covered with an excitonic layer [35], perovskite-exciton polaritons [36], and Mieexcitons in high-index dielectric NPs [37,38], possibly with a magneto-optical character [39]. ...
... For the calculation of the spectra, traditional Mie theory is obviously no longer applicable; we thus employ the nearest equivalent, namely the extended boundary condition method (EBCM) [61], which is still based on spherical-wave expansions. The simulation set-up and all convergence parameters are as described in Ref. [38]. We should note here that, within EBCM, the characterisation of modes in terms of multipoles is straightforward, because the matrix that connects the scattered to the incident field, though not diagonal, is almost always dominated by a single element with specific angular-momentum indices ℓ and m; alternatively, one can use Cartesian multipoles [62]. ...
... 30 In single-particle experiments, this is usually achieved by using nanoparticles of different dimensions. 31,32 As shown in Figure 3, we experimentally evaluate the evolution of the polariton-like hybridized modes in different TMD samples by tuning the a-SiNS:H sizes away from the optimal conditions in Figure 2. A clear anticrossing tendency is observed in both WSe 2 ( Figure 3a) and MoS 2 (Figure 3c) samples. As for WS 2 samples (Figure 3b), the anticrossing feature of LP is also well identified while the peak position of UP barely changes due to the existence of C exciton spectrally close to B exciton. ...
Two-dimensional exciton-polaritons in monolayer transition metal dichalcogenides (TMDs) exhibit practical advantages in valley coherence, optical nonlinearities, and even bosonic condensation owing to their light-emission capability. To achieve robust exciton-polariton emission, strong photon-exciton couplings are required at the TMD monolayer, which is challenging due to its atomic thickness. High-quality (Q) factor optical cavities with narrowband resonances are an effective approach but typically limited to a specific excitonic state of a certain TMD material. Herein, we achieve on-demand exciton-polariton emission from a wide range of TMDs at room temperature by hybridizing excitons with broadband Mie resonances spanning the whole visible spectrum. By confining broadband light at the TMD monolayer, our one type of Mie resonator on different TMDs enables enhanced light-matter interactions with multiple excitonic states simultaneously. We demonstrate multi-Rabi splittings and robust polaritonic photoluminescence in monolayer WSe2, WS2, and MoS2. The hybrid system also shows the potential to approach the ultrastrong coupling regime.
... Mirror cavities, the prototypical templates in cavity quantum electrodynamics [9,10], have long been employed as the most straightforward choice when considering atoms [11], while Bragg reflectors and photonic crystals constitute a natural option for artificial emitters such as quantum wells and dots [12,13]. More recently, excitons in molecular aggregates or transition-metal dichalcogenides (TMDs) [14] have been introduced as emitters with strong, collective (i.e., effective) dipole moments, leading to the emergence of, among others, plasmonic [15][16][17][18][19][20] and Mie-resonant [21][22][23][24] nanostructures as suitable effective cavities. What really determines the appropriateness of the cavity in all these endeavors is the linewidth of the emitter: the optical mode must be chosen to have a comparable linewidth, and the coupling strength must exceed the damping rates of the individual components * Present address: ICFO-Institut de Ciències Fotòniques, Barcelona Institute of Science and Technology, E-08860 Castelldefels (Barcelona), Spain. ...
... of gain it is possible to drive the exciton-cavity system to increase the number of Rabi oscillations that can be measured before damping prevails and the system completely loses its coherence. We revisit a recently introduced visibility measure [22] and provide a detailed gain-coupling map that quantifies the different coupling regimes; based on this, one can manipulate the dynamics of the system and accelerate or decelerate the Rabi oscillations to render their period more easily resolvable in experiments. Backtracking the visibility map, one can then extrapolate to infer the properties of the coupled system in the absence of gain. ...
... Such quality factors have already been introduced in the literature to deal with gainless strongly coupled systems [22,70], but here, we generalize their applicability to the case of cavities with gain. From Eq. (3), we straightforwardly obtain (while also assuming 2G |1 + |) ...
We propose an efficient approach for actively controlling the Rabi oscillations in nanophotonic emitter-cavity analogs based on the presence of an element with optical gain. Inspired by recent developments in parity-time (PT)-symmetry photonics, we show that nano- or microcavities where intrinsic losses are partially or fully compensated by an externally controllable amount of gain offer unique capabilities for manipulating the dynamics of extended (collective) excitonic emitter systems. In particular, we discuss how one can drastically modify the dynamics of the system, increase the overall occupation numbers, enhance the longevity of the Rabi oscillations, and even decelerate them to the point where their experimental observation becomes less challenging. Furthermore, we show that there is a specific gain value that leads to an exceptional point, where both the emitter and cavity occupation oscillate practically in phase, with occupation numbers that can significantly exceed unity. By revisiting a recently introduced Rabi-visibility measure, we provide robust guidelines for quantifying the coupling strength and achieving strong-coupling with adaptable Rabi frequency via loss compensation.
... Note that the strong coupling is not limited to two-dimensional materials. Two independent groups proposed to use an all-dielectric metasurface to realize the strong coupling of J-aggregated organic molecules [190,191]. The high-Q factor of collective surface lattice resonance directly results in a large Rabi-splitting around 200 meV for both TE and TM polarization. ...
... The integration of light emitters in silicon however, has been limited by the indirect nature of its band-gap. Si-based, light-emitting metasurfaces [190] have been demon-strated using more or less complex fabrication methods, such as spin coating colloidal quantum dots [191], or by atomic layer deposition [192] organic molecules [193], or coupling an emitting 2D material with sub-micrometric antennas [194,195,196]. These approaches do not embed the emitters in the core of the resonators, where the the electromagnetic field is stronger and electric-and magnetic-dipolar Mie modes can be tailored, providing more versatility for light management [133,197,198,199], as for instance shown for rare earth emitters coupled with plasmonic antennas [200] and light-emitting Si-nanocrystals in SiO 2 pillars [201]. ...
The aim of this thesis it to explore the potential of complex carbon impurities in silicon (G-centers) for applications in quantum technologies. This point defect was originally highlighted in carbon-rich Si samples undergoing high-energy electron irradiation followed by high temperature annealing. A key feature of G-centers is their infrared emission, matching the important optical telecommunications wavelength O-band spreading between 1260-1360 nm. Through my PhD work we have demonstrated that we are able to create individual G-centers by ion implantation in conventional silicon on insulator, isotopically purified 28Si on insulator, and embed these emitters in photonic nanostructures such as dielectric Mie resonators. The creation of single defects was demonstrated by measuring the anti-bunching in light intensity-correlation (second order auto-correlation function). We developed a low-resolution optical lithography and plasma etching method joined with solid state dewetting (defined in chapter 4.3) of monocrystalline, ultra-thin, silicon on insulator to form monocrystalline, atomically smooth, Mie resonators in well-controlled and large, periodic arrays. By integrating light emitting G-centers within the Si-based antennas we engineered the light emission by tuning carbon dose, beam energy and islands size in order to optimize the coupling between the emitters and the Mie resonances in space and frequency. Directional (Huygens-like) light emission at 120 K was demonstrated experimentally and confirmed by Finite Difference Time Domain simulations. We estimate that, with an optimal coupling of the G-centers emission with the resonant antennas, a collection efficiency of about 90% can be reached using a conventional objective lens. The integration of these telecom-frequency emitters in resonant antennas is relevant for their efficient exploitation in quantum optics applications and more generally to Si-based photonic metasurfaces.
... Harnessing polaritons at room temperature by spin-coating a thin film perovskite layer onto a processed silicon layer of a CMOS chip would be ideal to build future polaritonic devices. Recent studies have reported the surface lattice resonances (SLRs) of structured Si to achieve polaritons using organic molecules [33,34] and those of Ag structures using perovskites for conventional lasing [35]. However, owing to high refractive indexes of perovskites, perovskite-based polaritons on the patterned silicon platform or even broader SLR-supported system are yet to be investigated. ...
Owing to their high oscillator strength, binding energy, and low-cost fabrication, two-dimensional halide perovskites have recently gained attention as excellent materials for generating exciton-polaritons at room temperature. Unlike traditional materials used for polaritons, such as ZnO, GaAs, and GaN, halide perovskites exhibit great compatibility with matured CMOS technologies. However, no studies have reported perovskite-based polaritons on silicon platforms. Here, we numerically demonstrate the possibility of a polariton when a Si nanodisk array couples with a thin film of phenethylammonium lead iodide perovskite. An asymmetric lattice of thin Si nanodisks is used to generate surface lattice resonances from the coupling between the disk's electrical resonator and the lattice's diffracted waves. Polaritonic modes with high Rabi splitting values can be easily achieved for a large range of parameters. This Rabi splitting can be engineered by varying the ratio of electromagnetic energy confined within the Si disk and perovskite thin film. This study provides insight into nanophotonic structure design for CMOS-based optoelectronics, sensors, and polaritonic devices.
... Such composite architectures give rise to hybrid states, termed exciton polaritons or plexcitons, that combine the properties of both light and matter [36]. In addition to plexcitons, high-index dielectrics are more recently being considered as alternative environments for excitonic strong coupling, potentially as a way to surpass the hurdle of high Ohmic losses dominating metals, or to design novel polaritons with a magnetic character [37][38][39]. Strong coupling of a chiral excitonic material with an achiral resonator (e.g. a plasmonic NP) has already been shown to generate wide anticrossings in experimentally measured CD spectra [40]. ...
We introduce and theoretically analyze the concept of manipulating optical chirality via strong coupling of the optical modes of chiral nanostructures with excitonic transitions in molecular layers or semiconductors. With chirality being omnipresent in chemistry and biomedicine, and highly desirable for technological applications related to efficient light manipulation, the design of nanophotonic architectures that sense the handedness of molecules or generate the desired light polarization in an externally controllable manner is of major interdisciplinary importance. Here we propose that such capabilities can be provided by the mode splitting resulting from polaritonic hybridization. Starting with an object with well-known chiroptical response -- here, for a proof of concept, a chiral sphere -- we show that strong coupling with a nearby excitonic material generates two distinct frequency regions that retain the object's chirality density and handedness, which manifest most clearly through anticrossings in circular-dichroism or differential-scattering dispersion diagrams. These windows can be controlled by the intrinsic properties of the excitonic layer and the strength of the interaction, enabling thus the post-fabrication manipulation of optical chirality. Our findings are further verified via simulations of the circular dichroism of a realistic chiral architecture, namely a helical assembly of plasmonic nanospheres embedded in a resonant matrix.
