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A novel organic light emitting device intentionally couples emitter energy to the plasmon mode for increased device stability and converts plasmons to photons to improve device efficiency.

A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on the realization of hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the complex interplay between either system and the environment created by the color center host. Here we use an all-diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a high-critical-temperature superconducting film in the presence of a weak magnetic field. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductor-induced redistribution of charge carriers near the NV site. We build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the complex surface dynamics governing the spin coherence of shallow NVs while simultaneously paving the route to new forms of noise spectroscopy and imaging of superconductors.

We study theoretically effects of an anisotropic elastic strain on the exciton energy spectrum fine structure and optical selection rules in atom-thin crystals based on transition-metal dichalcogenides. The presence of strain breaks the chiral selection rules at the $\bm K$-points of the Brillouin zone and makes optical transitions linearly polarized. The orientation of the induced linear polarization is related to the main axes of the strain tensor. Elastic strain provides an additive contribution to the exciton fine structure splitting in agreement with experimental evidence obtained from uniaxially strained WSe$_2$ monolayer. The applied strain also induces momentum-dependent Zeeman splitting. Depending on the strain orientation and magnitude, Dirac points with a linear dispersion can be formed in the exciton energy spectrum. We provide a symmetry analysis of the strain effects and develop a microscopic theory for all relevant strain-induced contributions to the exciton fine structure Hamiltonian., Comment: 12 pages, 5 figures

The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2 phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2 and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics., In this work light and matter have been coupled in a strong interaction between exciton resonances and topological photonic bands. The authors herein demonstrate a Z2 spin-Hall topological polaritonic phase enabling new coupling schemes in valleytronics and spintronics.

Nonreciprocity and nonreciprocal optical devices play a vital role in modern photonic technologies by enforcing one-way propagation of light. Here, we demonstrate an all-optical approach to nonreciprocity based on valley-selective response in transition metal dichalcogenides (TMDs). This approach overcomes the limitations of magnetic materials and it does not require an external magnetic field. We provide experimental evidence of photoinduced nonreciprocity in a monolayer WS2 pumped by circularly polarized (CP) light. Nonreciprocity stems from valley-selective exciton population, giving rise to nonlinear circular dichroism controlled by CP pump fields. Our experimental results reveal a significant effect even at room temperature, despite considerable intervalley-scattering, showing promising potential for practical applications in magnetic-free nonreciprocal platforms. As an example, here we propose a device scheme to realize an optical isolator based on a pass-through silicon nitride (SiN) ring resonator integrating the optically biased TMD monolayer., Nonreciprocity is viewed as a useful feature for many future optical devices. Here, the authors observe all-optically-induced nonreciprocal dichroism in monolayer WS2, which is explained by valley-selective response.

Atomic-level defects in van der Waals (vdW) materials are essential building blocks for quantum technologies and quantum sensing applications. The layered magnetic semiconductor CrSBr is an outstanding candidate for exploring optically active defects owing to a direct gap in addition to a rich magnetic phase diagram including a recently hypothesized defect-induced magnetic order at low temperature. Here, we show optically active defects in CrSBr that are probes of the local magnetic environment. We observe spectrally narrow (1 meV) defect emission in CrSBr that is correlated with both the bulk magnetic order and an additional low temperature defect-induced magnetic order. We elucidate the origin of this magnetic order in the context of local and non-local exchange coupling effects. Our work establishes vdW magnets like CrSBr as an exceptional platform to optically study defects that are correlated with the magnetic lattice. We anticipate that controlled defect creation allows for tailor-made complex magnetic textures and phases with the unique ingredient of direct optical access., main: 12 pages, 5 figures; SI: 14 pages, 11 figures

The development of a controllable, selective, and repeatable etch process is crucial for controlling the layer thickness and patterning of two-dimensional (2D) materials. However, the atomically thin dimensions and high structural similarity of different 2D materials make it difficult to adapt conventional thin-film etch processes. In this work, we propose a selective, damage-free atomic layer etch (ALE) that enables layer-by-layer removal of monolayer WSe2 without altering the physical, optical, and electronic properties of the underlying layers. The etch uses a top-down approach where the topmost layer is oxidized in a self-limited manner and then removed using a selective etch. Using a comprehensive set of material, optical, and electrical characterization, we show that the quality of our ALE processed layers is comparable to that of pristine layers of similar thickness. The ALE processed WSe2 layers preserve their bright photoluminescence characteristics and possess high room-temperature hole mobilities of 515 cm2/V·s, essential for fabricating high-performance 2D devices. Further, using graphene as a testbed, we demonstrate the fabrication of ultra-clean 2D devices using a sacrificial monolayer WSe2 layer to protect the channel during processing, which is etched in the final process step in a technique we call sacrificial WSe2 with ALE processing (SWAP). The graphene transistors made using the SWAP technique demonstrate high room-temperature field-effect mobilities, up to 200,000 cm2/V·s, better than previously reported unencapsulated graphene devices.

Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for studying fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening with an effective electron mass ratio of $m^e_X/m^e_Y \sim 50$. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability and a Fano resonance from a van Hove singularity of similar strength of metallic carbon nanotubes. Moreover, due to the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D correlated many-body physics in the presence of magnetic order., main: 16 pages, 5 figures; SI: 15 pages, 9 figures

Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances have yet to be found. Here we report strong light-matter coupling in $\textrm{NiPS}_3$, a van der Waals antiferromagnet with highly correlated electronic degrees of freedom. A previously unobserved class of polaritonic quasiparticles emerges from the strong coupling between its spin-correlated excitons and the photons inside a microcavity. Detailed spectroscopic analysis in conjunction with a microscopic theory provides unique insights into the origin and interactions of these exotic magnetically coupled excitations. Our work introduces van der Waals magnets to the field of strong light-matter physics and provides a path towards the design and control of correlated electron systems via cavity quantum electrodynamics.

The field of plasmonics, which studies the resonant interactions of electromagnetic waves and free electrons in solid-state materials1, has yet to be put to large-scale commercial application2 owing to the large amount of loss that usually occurs in plasmonic materials3. Organic light-emitting devices (OLEDs)4-7 have been incorporated into billions of commercial products because of their good colour saturation, versatile form factor8 and low power consumption9, but could still be improved in terms of efficiency and stability. Although OLEDs incorporating organic phosphors achieve an internal charge-to-light conversion of unity10, their refractive index contrast reduces the observable fraction of photons outside the device to around 25 per cent11-13. Further, during OLED operation, a localized buildup of slow-decaying14 triplet excitons and charges15 gradually reduces the brightness of the device in a process called ageing16,17, which can result in 'burn-in' effects on the display. Simultaneously improving device efficiency and stability is of paramount importance for OLED technology. Here we demonstrate an OLED that uses the decay rate enhancement18 of a plasmonic system to increase device stability, while maintaining efficiency by incorporating a nanoparticle-based out-coupling scheme to extract energy from the plasmon mode. Using an archetypal phosphorescent emitter, we achieve a two-fold increase in operational stability at the same brightness as a reference conventional device while simultaneously extracting 16 per cent of the energy from the plasmon mode as light. Our approach to increasing OLED stability avoids material-specific designs19-22 and is applicable to all commercial OLEDs that are currently used for lighting panels, televisions and mobile displays.

Integration of quantum emitters in photonic structures is an important step in the broader quest to generate and manipulate on-demand single photons via compact solid-state devices. Unfortunately, implementations relying on material platforms that also serve as the emitter host often suffer from a tradeoff between the desired emitter properties and the photonic system practicality and performance. Here, we demonstrate “pick and place” integration of a Si3N4 microdisk optical resonator with a bright emitter host in the form of ∼20-nm-thick hexagonal boron nitride (hBN). The film folds around the microdisk maximizing contact to ultimately form a hybrid hBN/Si3N4 structure. The local strain that develops in the hBN film at the resonator circumference deterministically activates a low density of defect emitters within the whispering gallery mode volume of the microdisk. These conditions allow us to demonstrate cavity-mediated out-coupling of emission from defect states in hBN through the microdisk cavity modes. Our results pave the route toward the development of chip-scale quantum photonic circuits with independent emitter/resonator optimization for active and passive functionalities.

Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances are yet to be found. Here, we report strong light-matter coupling in NiPS

We use density functional theory (DFT) to explore the physical properties of an $Er_{ W}$ point defect in monolayer $WS_{ 2}$. Our calculations indicate that electrons localize at the dangling bonds associated with a tungsten vacancy ($V_{W}$) and at the $Er^{ 3+}$ ion site, even in the presence of a net negative charge in the supercell. The system features a set of intra-gap defect states, some of which are reminiscent of those present in isolated $Er^{ 3+}$ ions. In both instances, the level of hybridization is low, i.e., orbitals show either strong Er or W character. Through the calculation of the absorption spectrum as a function of wavelength, we identify a broad set of transitions, including one possibly consistent with the $Er^{ 3+}$ $4I_{ 15/2} \rightarrow 4I_{ 13/2}$ observed in other hosts. Combined with the low native concentration of spin-active nuclei as well as the two-dimensional nature of the host, these properties reveal $Er:WS_{ 2}$ as a potential platform for realizing spin qubits that can be subsequently integrated with other nanoscale optoelectronic devices.

A hitherto unobserved three-body coupled composite of excitons, photons and spins is created by strong light-matter coupling in a van der Waals magnetic insulator hosting spin-correlated excitonic excitations [1]. (c) 2022 The Authors(s)

Strong light–matter coupling results in the formation of hybrid half-light half-matter excitations with modified energy levels. The strong coupling of excitons with photons in organic molecular sys...

A quasi-one-dimensional organic semiconductor, hepta(p-phenylene vinylene) (HPV), was incorporated into a DNA tensegrity triangle motif using a covalent strategy. 3D arrays were self-assembled from an HPV-DNA pseudo-rhombohedron edge by rational design and characterized by X-ray diffraction. Templated by the DNA motif, HPV molecules exist as single-molecule fluorescence emitters at the concentration of 8 mM within the crystal lattice. The anisotropic fluorescence emission from HPV-DNA crystals indicates HPV molecules are well aligned in the macroscopic 3D DNA lattices. Sophisticated nanodevices and functional materials constructed from DNA can be developed from this strategy by addressing functional components with molecular accuracy.

Description, Nanowires induce mechanical deformations in monolayer semiconductors, creating potential channels that guide optical excitations., Strain engineering is a powerful tool in designing artificial platforms for high-temperature excitonic quantum devices. Combining strong light-matter interaction with robust and mobile exciton quasiparticles, two-dimensional transition metal dichalcogenides (2D TMDCs) hold great promise in this endeavor. However, realizing complex excitonic architectures based on strain-induced electronic potentials alone has proven to be exceptionally difficult so far. Here, we demonstrate deterministic strain engineering of both single-particle electronic bandstructure and excitonic many-particle interactions. We create quasi-1D transport channels to confine excitons and simultaneously enhance their mobility through locally suppressed exciton-phonon scattering. Using ultrafast, all-optical injection and time-resolved readout, we realize highly directional exciton flow with up to 100% anisotropy both at cryogenic and room temperatures. The demonstrated fundamental modification of the exciton transport properties in a deterministically strained 2D material with effectively tunable dimensionality has broad implications for both basic solid-state science and emerging technologies.

Description, We demonstrate brightening of dark molecular isomeric states via strong coupling in optical microcavities., Polaritons in organic systems has shown the potential to modify chemical properties and to mediate long-range energy transfer between individual chromophores, among other capabilities. Here, we demonstrate that strong coupling and formation of organic exciton-polaritons can be used to selectively tune the isomer emission of organic molecules. By taking advantage of their delocalized and hybrid character, polaritons emerging in the strong coupling regime open a new relaxation pathway that allows for an efficient funneling of the excitation between the molecular isomers. We implement this by strong coupling to trans-DCS (E-4-dimethylamino-4′cyanostilbene)molecules, which present two isomers in different amounts when immersed in a polymer matrix. Thanks to this new relaxation pathway, the photoexcitation that is first shared by the common polaritonic mode is then selectively funneled to the excited states of one of the isomers, recognizing pure emission from the isomeric states that do not contribute to emission under normal conditions.

Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS$_2$ alleviates this issue owing to their hybridization of interlayer charge transfer exciton and intralayer B exciton. Here we demonstrate the formation of dipolar exciton polaritons in bilayer MoS$_2$ resulting in unprecedented nonlinear interaction strengths. A ten-fold increase in nonlinearity is observed for the interlayer dipolar excitons compared to the conventional A excitons. These highly nonlinear dipolar polaritons will likely be a frontrunner in the quest for solid-state quantum nonlinear devices., 32 pages, 14 figures

The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics. However, there is no consensus on the types of molecular systems whose dynamics can be modified using strong coupling. These open questions stem from persistent uncertainties concerning the lifetime and conversion dynamics of exciton-polaritons and localized excited states as well as the proper way to measure such interactions in the time-domain. Here, we provide a framework for measuring dynamical interactions between exciton-polaritons and a diverse manifold of singlet, triplet, and multiexciton states, using a model molecular spin conversion (singlet fission) system that is strongly coupled to an optical microcavity. In addition to the usual population dynamics, transient optical measurements on microcavities are sensitive to transient modifications of the exciton-polariton transition energies, exciton-photon coupling conditions, and thermal excitations of the cavity mirrors.

Single photon sources (quantum emitters) are a key building block for emerging quantum technologies. Especially attractive for quantum photonic circuitry is the prospect of integrating such sources with conventional photonic structures such as resonators and waveguides. In this talk, we will first present our work on realizing single photon emitters (SPEs) in hexagonal boron nitride (hBN), a van der Waals material, via strain engineering. Following this we will discuss the coupling of such SPEs to silicon nitride microdisk resonators and to plasmonic surface lattice resonances. Prospects of realizing electrically driven SPEs using few layer hBN placed in van der Waals heterostructures will also be discussed.

Two-dimensional van der Waals (vdW) materials have emerged as a very attractive class of optoelectronic material due to their extraordinarily strong interaction with light. In this talk we will present our recent work on strong light-matter coupling and control of the excitons in 2D transition metal dichalcogenides. Specifically, we will discuss nonlinear optical response of the strongly coupled states, control of chiral light-matter interaction in these materials using metamaterials, and the use of strain and artifical gauge fields to control transport and valley properties of the excitons.

Spin-forbidden intravalley dark excitons in tungsten-based transition-metal dichalcogenides (TMDCs), because of their unique spin texture and long lifetime, have attracted intense research interest. Here, we show that we can control the dark exciton electrostatically by dressing it with one free electron or free hole, forming the dark trions. The existence of the dark trions is suggested by the unique magneto-photoluminescence spectroscopy pattern of the boron nitride (BN)-encapsulated monolayer WSe2 device at low temperature. The unambiguous evidence of the dark trions is further obtained by directly resolving the radiation pattern of the dark trions through back focal plane imaging. The dark trions possess a binding energy of ∼15 meV, and they inherit the long lifetime and large g-factor from the dark exciton. Interestingly, under the out-of-plane magnetic field, dressing the dark exciton with one free electron or hole results in distinctively different valley polarization of the emitted photon, as a result of the different intervalley scattering mechanism for the electron and hole. Finally, the lifetime of the positive dark trion can be further tuned from ∼50 ps to ∼215 ps by controlling the gate voltage. The gate-tunable dark trions usher in new opportunities for excitonic optoelectronics and valleytronics.

Transition Metal Dichalcogenides (TMDCs) have been in the limelight for the past decade as a candidate for several optoelectronic devices, and as a versatile test bed for various fundamental light-matter interaction phenomena thanks to their exceptional linear optical properties arising from their large binding energy, strong spin-orbit coupling and valley physics in the monolayer (ML) limit. They also boast strong non-linear properties fortied by excitonic responses in these systems. However, the strong second order non-linear responses are mostly restricted to the ML limit owing to crystal symmetry requirements, posing several limitations in terms of smaller interaction length and lower damage threshold. Here we demonstrate a self-hybridized exciton-polariton system in bulk WSe2 that allows us to relax the crystal symmetry rules that govern second order non-linearities. The demonstrated polariton system shows intense Second Harmonic Generation (SHG) when the fundamental wavelength is resonant with the lower polariton, with an efficiency comparable to the one from a ML WS2 when excited at the same fundamental wavelength and intensity. We model this phenomenon by considering a system with alternating second- order susceptibilities under an asymmetric electric field profile determined by the polariton mode. Helicity resolved polarization experiments show very similar non-linear response as the one from a ML where the helicity of the SHG flips with respect to the fundamental harmonic. This polaritonic system offers a platform to leverage robust second order non-linear response from centrosymmetric systems, while at the same time allowing access to third-order non-linearity inherent in strongly coupled systems.

We demonstrate a method to implement a Zeeman term to the 2D-Ising Hamiltonian in a spatial Ising machine. An NP-complete problem of the 2D-Ising spin-glass in an external magnetic field is studied.

Optical antennas made of low-loss dielectrics have several advantages over plasmonic antennas, including high radiative quantum efficiency, negligible heating, and excellent photostability. However, due to weak spatial confinement, conventional dielectric antennas fail to offer light-matter interaction strengths on par with those of plasmonic antennas. We propose here an all-dielectric antenna configuration that can support strongly confined modes ($V\ensuremath{\sim}{10}^{\ensuremath{-}4}{\ensuremath{\lambda}}_{0}^{3}$) while maintaining unity antenna quantum efficiency. This configuration consists of a high-index pillar structure with a transverse gap that is filled with a low-index material, where the contrast of indices induces a strong enhancement of the electric field perpendicular to the gap. We provide a detailed explanation of the operational principle of such photonic gap antennas (PGAs) based on the dispersion relation of symmetric and asymmetric horizontal slot waveguides. To discuss the properties of PGAs, we consider silicon pillars with air or the polymer CYTOP as the gap material. We show by full-wave simulations that PGAs with an emitter embedded in the gap can enhance the spontaneous emission rate by a factor of approximately $1000$ for air gaps and approximately $400$ for CYTOP gaps over a spectral bandwidth of $\mathrm{\ensuremath{\Delta}}\ensuremath{\lambda}\ensuremath{\approx}300\phantom{\rule{0.2em}{0ex}}\mathrm{nm}$ at $\ensuremath{\lambda}=1.25\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}\mathrm{m}$. Furthermore, the PGAs can be designed to provide unidirectional out-of-plane radiation across a substantial portion of their spectral bandwidth. This is achieved by setting the position of the gap at an optimized off-centered position of the pillar so as to properly break the vertical symmetry of the structure. We also demonstrate that, when acting as receivers, PGAs can lead to a near-field intensity enhancement by a factor of approximately $3000$ for air gaps and approximately $1200$ for CYTOP gaps.

We study thermalization of exciton-polaritons in 2D hybrid organic-inorganic perovskites strongly coupled to a planar microcavity. The integrated PL exhibits a bottleneck effect and the extracted lattice temperature shows cooling behavior of up to 35 meV.

The development of a controllable, selective, and repeatable etch process is crucial for controlling the layer thickness and patterning of two-dimensional (2D) materials. However, the atomically thin dimensions and high structural similarity of different 2D materials make it difficult to adapt conventional thin-film etch processes. In this work, we propose a selective, damage-free atomic layer etch (ALE) that enables layer-by-layer removal of monolayer WSe

Luminescence arising from $\ensuremath{\beta}$ decay of radiotracers has attracted much interest recently as a viable in vivo imaging technique. The emitted Cerenkov radiation can be directly detected by high-sensitivity cameras or used to excite highly efficient fluorescent dyes. Here we investigate the enhancement of visible and infrared emission driven by $\ensuremath{\beta}$ decay of radioisotopes in the presence of a hyperbolic nanocavity. By means of a transfer-matrix approach, we obtain quasianalytic expressions for the fluorescence-enhancement factor at the dielectric core of the metalodielectric cavity, and report a 100-fold amplification in periodic structures. A particle-swarm optimization of the layered shell geometry reveals that enhancement of up to $10\phantom{\rule{0.1em}{0ex}}000$-fold is possible because of the hybridization and spectral overlap of whispering-gallery and localized-plasmon modes. Our findings may find application in nuclear-optical medical imaging, as they provide a strategy for the use of highly energetic gamma rays, Cerenkov luminescence, and visible and near-infrared fluorescence through the same nanotracer.

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${g}_{{pol}-{pol}}^{2s} \sim 46.4\pm 13.9\,\mu {eV}\mu {m}^{2}$$\end{document}gpol−pol2s~46.4±13.9μeVμm2 which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies., Here, the authors show the formation of exciton-polaritons with enhanced nonlinear response using excited excitonic Rydberg states in monolayer WSe2 embedded in a microcavity.

The field of plasmonics, which studies the resonant interactions of electromagnetic waves and free electrons in solid-state materials

We report enhanced second harmonic generation (SHG) from centrosymmetric bulk WSe2. This enhancement arises due to pumping in resonance with the Exciton-Polariton modes formed in self-hybridized bulk WSe2.

We demonstrate significant enhancement (> 40%) in valley coherence of localized excitons in monolayer WS2 via strain engineering. The observed enhancement is attributed to the suppression of inter valley scattering due to strain induced potential.

We demonstrate room-temperature ultralong-range transport >80 pm of exciton- polaritons in a disordered organic thin-film using a one-sided distributed Bragg reflector, which is orders of magnitude larger than expected for excitons in disordered systems.

The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before such systems can be realized, it is essential to address the open questions concerning the nature and strength of electronic interactions between exciton-polaritons and localized excited states in chemical system as well as the proper way to measure such interactions. Here, we use transient optical spectroscopy to investigate dynamical interactions between exciton-polaritons, singlet excitons, and triplet excitons in a molecular singlet fission system that is strongly coupled to an optical microcavity. We identify some of the major limitations to modify molecular dynamics in the strong coupling regime. Simultaneous excitation of cavity polaritons and 'reservoir' states, defined as dark polaritons and dark excitons (e.g. triplets) from coupled molecules and excitons from uncoupled molecules, always occurs. In addition, slow conversion from reservoir states to cavity polaritons results in minimal changes to the overall population dynamics. Furthermore, we demonstrate how in addition to the usual population dynamics, transient optical measurements on microcavities reveal information pertaining to modification of the exciton-polariton transition energies due to changes in the population of molecular excited states and the exciton-photon coupling conditions. As a consequence of weak interactions between reservoir states and cavity polaritons, judicious design considerations are required to achieve modified chemical dynamics, necessitating the use of molecular systems with long excited-state lifetimes or strong coupling approaches that require a small number of molecules.

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical responses can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron–phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the cavity polaritons to be promising as sensitive probes of non-equilibrium phenomena.

We demonstrate valley dependent long-range propagation features in a polariton fluid formed via coupling WS2 excitons to Bloch surface waves at room temperatures.