Collective Mie Exciton-Polaritons in an Atomically Thin Semiconductor
Shaojun Wang, T. V. Raziman, Shunsuke Murai, Gabriel W. Castellanos, Ping Bai, Anton Matthijs Berghuis, Rasmus H. Godiksen, Alberto G. Curto, Jaime Gómez Rivas
Optically induced Mie resonances in dielectric nanoantennas feature low dissipative losses and large resonant enhancement of both electric and magnetic fields. They offer an alternative platform to plasmonic resonances to study light-matter interactions from the weak to the strong coupling regimes. Here, we experimentally demonstrate the strong coupling of bright excitons in monolayer WS$_2$ with Mie surface lattice resonances (Mie-SLRs). We resolve both electric and magnetic Mie-SLRs of a Si nanoparticle array in angular dispersion measurements. At the zero detuning condition, the dispersion of electric Mie-SLRs (e-SLRs) exhibits a clear anti-crossing and a Rabi-splitting of 32 meV between the upper and lower polariton bands. The magnetic Mie-SLRs (m-SLRs) nearly cross the energy band of excitons. These results suggest that the field of m-SLRs is dominated by out-of-plane components that do not efficiently couple with the in-plane excitonic dipoles of the monolayer WS$_2$. In contrast, e-SLRs in dielectric nanoparticle arrays with relatively high quality factors (Q $\sim$ 120) facilitate the formation of collective Mie exciton-polaritons, and may allow the development of novel polaritonic devices which can tailor the optoelectronic properties of atomically thin two-dimensional semiconductors.
We implement externally excited ZnO Mie resonators in a framework of a generalized Hubbard Hamiltonian to investigate the lifetimes of excitons and exciton-polaritons out of thermodynamical equilibrium. Our results are derived by a Floquet-Keldysh-Green's formalism with Dynamical Mean Field Theory (DMFT) and a second order iterative perturbation theory solver (IPT). We find that the Fano resonance which originates from coupling of the continuum of electronic density of states to the semiconductor Mie resonator yields polaritons with lifetimes between 0.6 ps and 1.45 ps. These results are compa…
Light-matter interactions at the nanoscale constitute a fundamental ingredient for engineering applications in nanophotonics and quantum optics. To this regard electromagnetic Mie resonances excited in high-refractive index dielectric nanoparticles have recently attracted interest because of their lower losses and better control over the scattering patterns compared to their plasmonic metallic counterparts. The emergence of several resonances in those systems results in an overall high complexity, where the electric and magnetic dipoles have significant overlap in the case of spherical symmetr…
Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been in the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist ang…
Monolayer transition metal dichalcogenides (TMDCs) have recently been proposed as a unique excitonic platform for advanced optical and electronic functionalities. However, in spite of intense research efforts, it has been largely overlooked that, in addition to displaying rich exciton physics, TMDCs also possess a very high refractive index. This opens a possibility to utilize these materials for constructing resonant nanoantennas based on subwavelength geometrical modes. Here we show that nanodisks fabricated from exfoliated multilayer WS$_2$ support distinct Mie resonances and so-called anap…
Nonlinear optical effects such as four-wave mixing and generation of squeezed light are ubiquitous in optical devices and light sources. For new devices operating at low optical power, the resonant nonlinearity arising from the two-photon sensitive bound biexciton in a semiconductor microcavity is an interesting prospective platform. Due to the particularly strong Coulomb interaction in atomically thin semiconductors, these materials have strongly bound biexcitons and operate in the visible frequency range of the electromagnetic spectrum. To remove the strong pump laser from the generated ligh…
The interference of polariton guiding modes propagating through "traffic circle" waveguides composed of dielectric spherical particles is investigated. The dependence of intensity of the wave on the position of the particle was studied using the multisphere the Mie scattering formalism. We show that if the frequency of light belongs to the passband of the waveguide, electromagnetic waves may be considered as two optical beams running along a circle in opposite directions and interfering with each other. Indeed, the obtained intensity behavior can be represented as a simple superposition of two…
Plasmon polaritons in van der Waals (vdW) materials hold promise for next-generation photonics. The ability to deterministically imprint spatial patterns of high carrier density in cavities and circuitry with nanoscale features underlies future progress in nonlinear nanophotonics and strong light-matter interactions. Here, we demonstrate a general strategy to atomically imprint low-loss graphene plasmonic structures using oxidation-activated charge transfer (OCT). We cover graphene with a monolayer of WSe$_2$, which is subsequently oxidized into high work-function WOx to activate charge transf…
We present all-dielectric polaritonic metasurfaces consisting of properly sculptured cylinders to sustain the dynamic anapole, i.e. a non-radiating alternating current distribution. One way for the anapole to emerge, is by combining modes based on the first and the fourth Mie resonance of a cylinder made of high permittivity LiTaO$_3$ for operation in the low THz. The circular cross-section of each cylinder varies periodically along its length in a binary way, from small to large, while its overall circular symmetry has to be broken in order to remove parasitic magnetic modes. Small cross-sect…
Atomically thin transition metal dichalcogenides possess valley dependent functionalities that are usually available only at crogenic temperatures, constrained by various valley depolarization scatterings. The formation of exciton polaritons by coherently superimposing excitons and microcavity photons potentially harnesses the valley polarized polariton polariton interactions for novel valleytronics devices. Robust EPs have been demonstrated at room temperature in TMDs microcavity, however, the coherent polariton lasing and condensation remain elusive. Herein, we demonstrate for the first time…
Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form quasiparticles known as polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with cavity-assisted hyperspectral imaging. Using extended WS$_2$ monolayers, we establish the regime of strong coupling with a scanning microcavity to map out polariton pro…
The emergence of spatial and temporal coherence of light emitted from solid-state systems is a fundamental phenomenon, rooting in a plethora of microscopic processes. It is intrinsically aligned with the control of light-matter coupling, and canonical for laser oscillation. However, it also emerges in the superradiance of multiple, phase-locked emitters, and more recently, coherence and long-range order have been investigated in bosonic condensates of thermalized light, as well as in exciton-polaritons driven to a ground state via stimulated scattering. Here, we experimentally show that the in…
Near-field mapping has been widely used to study hyperbolic phonon-polaritons in van der Waals crystals. However, an accurate measurement of the polaritonic loss remains challenging because of the inherent complexity of the near-field signal and the substrate-mediated loss. Here we demonstrate that large-area monocrystalline gold flakes, an atomically-flat low-loss substrate for image polaritons, provide a platform for precise near-field measurement of the complex propagation constant of polaritons in van der Waals crystals. As a topical example, we measure propagation loss of the image phonon…
Optimizing strong light-matter coupling of plasmonic lattices and monolayer semiconductors
Ludwig-Maximilians-Universität München（慕尼黑大学）；Technische Universität Darmstadt（达姆施塔特工业大学）；University of Basel（巴塞尔大学）；National Institute for Materials Science（国立材料研究所）；Karadeniz Technical University（卡拉登技术大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）
Monolayer transition metal dichalcogenides (TMDs) are the first truly two-dimensional (2D) semiconductor, providing an excellent platform to investigate light-matter interaction in the 2D limit. Apart from fundamental scientific exploration, this material system has attracted active research interest in the nanophotonic devices community for its unique optoelectronic properties. The inherently strong excitonic response in monolayer TMDs can be further enhanced by exploiting the temporal confinement of light in nanophotonic structures. Dielectric metasurfaces are one such two-dimensional nanoph…
Engineering non-linear hybrid light-matter states in tailored optical lattices is a central research strategy for the simulation of complex Hamiltonians. Excitons in atomically thin crystals are an ideal active medium for such purposes, since they couple strongly with light and bear the potential to harness giant non-linearities and interactions while presenting a simple sample-processing and room temperature operability. We demonstrate lattice polaritons, based on an open, high-quality optical cavity, with an imprinted photonic lattice strongly coupled to excitons in a WS$_{2}$ monolayer. We …
A deterministic and scalable array of single photon nonlinearities in the solid state holds great potential for both fundamental physics and technological applications, but its realization has proved extremely challenging. Despite significant advances, leading candidates such as quantum dots and group III-V quantum wells have yet to overcome their respective bottlenecks in random positioning and weak nonlinearity. Here we consider a hybrid light-matter platform, marrying an atomically thin two-dimensional material to a photonic crystal cavity, and analyze its second-order coherence function. W…
Exciton polaritons in atomically-thin transition metal dichalcogenide crystals (monolayer TMDCs) have emerged as a promising candidate to enable topological transport, ultra-efficient laser technologies, and collective quantum phenomena such as polariton condensation and superfluidity at room temperature. However, integrating monolayer TMDCs into high-quality planar microcavities to achieve the required strong coupling between the cavity photons and the TMDC excitons (bound electron-hole pairs) has proven challenging. Previous approaches to integration had to compromise between various adverse…
We report thorough measurements of surface plasmon polaritons (SPPs) running along nearly perfect air-gold interfaces formed by atomically flat surfaces of chemically synthesized gold monocrystals. By means of amplitude- and phase-resolved near-field microscopy, we obtain their propagation length and effective mode index at visible wavelengths (532, 594, 632.8, 729, and 800 nm). The measured values are compared with the values obtained from the dielectric functions of gold that are reported in literature. Importantly, a reported dielectric function of monocrystalline gold implies $\sim 1.5$ ti…
