All-optical logic has the potential to overcome the operation speed barrier that has persisted in electronic circuits for two decades. However, the development of scalable architectures has been prevented so far by the lack of materials with sufficiently strong nonlinear interactions needed to realize compact and efficient ultrafast all-optical switches with optical gain. Microcavities with embedded organic material in the strong light-matter interaction regime have recently enabled all-optical transistors operating at room temperature with picosecond switching times. However, the vertical cavity geometry, which is predominantly used in polaritonics, is not suitable for complex circuits with on-chip coupled transistors. Here, by leveraging state-of-the-art silicon photonics technology, we have achieved exciton-polariton condensation at ambient conditions in fully integrated high-index contrast sub-wavelength grating microcavities filled with a π-conjugated polymer as optically active material. We demonstrate ultrafast all-optical transistor action by coupling two resonators and utilizing seeded polariton condensation. With a device area as small as 2 × 2 µm2, we realize picosecond switching and amplification up to 60x, with extinction ratio up to 8:1. This compact ultrafast transistor device with in-plane integration is a key component for a scalable platform for all-optical logic circuits that could operate two orders of magnitude faster than electronic counterparts. Using integrated silicon high-contrast sub-wavelength gratings and organic cavity exciton-polaritons at room temperature, we realize all-optical transistor action with picosecond switching and amplification, as well as ultracompact footprint.
Single photons in Laguerre-Gaussian (LG) beams, which carry orbital angular momentum (OAM), could enable more robust and efficient photonic quantum communication and information processing, as well as enhanced sensitivity in quantum metrology and imaging. However, as most implementations are indirect or require additional mode-shaping elements, the direct generation of single photons with OAM has received growing interest. Colloidal lead halide perovskite quantum dots (QDs) have recently emerged as a versatile material that can produce indistinguishable single photons quasi-deterministically at a high rate. Here, we integrate single CsPbBr3 QDs into an open Fabry-Perot microcavity with a nanofabricated Gaussian-shaped deformation, demonstrating Purcell-enhanced single-photon generation into individual cavity modes with up to 18.1 ± 0.2 times accelerated decay, down to tens of picoseconds. By in situ tuning of the cavity resonance, we can selectively couple a single QD to different LG modes and observe the spatial patterns of the generated single-photon beams emitted from the cavity. Our findings may guide the development of high-photon-rate sources that directly generate single-photon LG beams for advanced quantum photonic applications.
Interactions between emitters can create cooperative effects that alter light emission. In superfluorescence (SF), excited dipoles couple coherently and radiate collectively, requiring low energetic disorder and strong temporal coherence. Conversely, amplified spontaneous emission results from stimulated amplification and does not require temporal coherence but, unlike SF, sufficient propagation for optical gain. Caesium lead halide perovskite nanocrystals exhibit both amplified spontaneous emission (in disordered films) and SF (in ordered assemblies); however, the connections between these regimes remain unclear. Here we demonstrate that temperature and excitation density can drive the transition between both regimes in a thin film of giant CsPbBr 3 perovskite nanocrystals. At temperatures below 45 K, excitonic SF was observed, whereas above a transition range between 45 K and 100 K, amplified spontaneous emission prevails but requires increased optical excitation and emitter density. Our results work out the different collective effects present in lead halide perovskites, providing fundamental insights into cooperative phenomena and guidance for the development of compact and bright (quantum) light sources.
The exploitation of the strong light-matter coupling regime and exciton-polariton condensates has emerged as a compelling approach to introduce strong interactions and nonlinearities into numerous photonic applications. The use of colloidal semiconductor quantum dots with strong three-dimensional confinement as the active material in optical microcavities would be highly advantageous due to their versatile structural and compositional tunability and wet-chemical processability, as well as potentially enhanced, confinement-induced polaritonic interactions. Yet, to date, exciton-polariton condensation in a microcavity has neither been achieved with epitaxial nor with colloidal quantum dots. Here, we demonstrate room-temperature polariton condensation in a thin film of monodisperse, colloidal CsPbBr3 quantum dots, placed in a tunable optical resonator with a Gaussian-shaped deformation serving as wavelength-scale potential well for polaritons. The onset of polariton condensation under pulsed optical excitation is manifested in emission by its characteristic superlinear intensity dependence, reduced linewidth, blueshift, and extended temporal coherence.
Exciton-polariton microcavity arrays have emerged as a promising semiconductor-based platform for analog simulations of model Hamiltonians and topological effects. To study a variety of Hamiltonians and investigate their properties, it is essential to have highly configurable and easily engineerable structures with low disorder. Here, we demonstrate in situ tunable, room-temperature polariton condensation in individual states of a Su-Schrieffer-Heeger topological lattice by using an open-cavity configuration with an organic polymer layer. Changing the cavity length in combination with vibron-mediated relaxation in the polymer allows us to achieve selective polariton condensation into different states of the band structure, unveiled by nonlinear emission, linewidth narrowing, energy blue shift, and extended macroscopic coherence. Furthermore, we engineer the bandgap and the edge state localization by adjusting the interaction between adjacent lattice sites. Our results demonstrate the versatility and accuracy of the platform for the investigation of quantum fluids in complex potential landscapes and topological effects at room temperature.
A central challenge for advancing polariton-based circuits is the controlled and scalable coupling of individual condensates. Existing approaches based on etched or epitaxially grown microcavities are fabrication-intensive and restrict in-plane coupling. To overcome these limitations, we introduce a lithographically defined silicon-based platform of high-contrast grating (HCG) microcavities with a ladder-type π-conjugated polymer. In this system, doublet cavities exhibit mode hybridization into bonding and antibonding states, where coupling is mediated across shared HCG mirrors. Extending the design to arrays, N-coupled condensates exhibit systematic red-shifts of the condensate energy, due to delocalization, and a progressive threshold reduction, consistent with extended binding modes. Our experimental results are quantitatively supported by transition-matrix multi-scattering simulations, together with tight-binding modelling. First-order coherence measurements using Michelson interferometry confirm the existence of spatially extended condensates with exponentially decaying temporal coherence. Altogether, these results establish a scalable route toward integrated polariton devices and quantum photonic networks.
We study the formation of topological defects via the Kibble-Zurek mechanism in a polariton supersolid in a liquid crystal microcavity with tunable Rashba-Dresselhaus spin-orbit coupling. We predict analytically two different scalings in the slow- and fast-quench regimes, and confirm these predictions numerically. We also present experimental results for the slow-quench regime, demonstrating an original Kibble-Zurek scaling exponent η_KZM=1.0± 0.2
The tunability of individual coupling amplitudes in photonic lattices is highly desirable for photonic Hamiltonian engineering and for studying topological transitions in situ. In this work, we demonstrate the tunneling control between individual lattice sites patterned inside an optical microcavity. The tuning is achieved by applying a voltage to a liquid crystal microcavity possessing photonic Rashba-Dresselhaus spin-orbit coupling. This type of spin-orbit coupling emerges due to the high birefringence of the liquid crystal material and constitutes an artificial gauge field for photons. The proposed technique can be combined with strong-light matter coupling and non-Hermitian physics already established in liquid crystal microcavities.
Highly ordered nanocrystal (NC) assemblies, namely, superlattices (SLs), have been investigated as materials for optical and optoelectronic devices due to their unique properties based on interactions among neighboring NCs. In particular, lead halide perovskite NC SLs have attracted significant attention owing to their extraordinary optical characteristics of individual NCs and collective emission processes like superfluorescence (SF). So far, the primary method for preparing perovskite NC SLs has been the drying-mediated self-assembly method, in which the colloidal NCs spontaneously assemble into SLs during solvent evaporation. However, this method lacks controllability because NCs form random-sized SLs at random positions on the substrate, rendering NC assemblies in conjunction with device structures, such as photonic waveguides or microcavities, challenging. Here, we demonstrate template-assisted self-assembly to deterministically place perovskite NC SLs and control their geometrical properties. A solution of CsPbBr3 NCs is drop-casted on a substrate with lithographically defined hollow structures. After solvent evaporation and removal of excess NCs from the substrate surface, NCs remain only in the templates, thereby defining the position and size of these NC assemblies. We performed photoluminescence (PL) measurements on these NC assemblies and observed signatures of SF, similar to those in spontaneously assembled SLs. Our findings are crucial for optical devices that harness embedded perovskite NC assemblies and enable fundamental studies on how these collective effects can be tailored through the SL geometry.
A sample refinement strategy suitable for accurately locating a large number of poles is introduced. We tie the AAA algorithm into an automatic differentiation framework to efficiently differentiate multi-scattering resonance calculations. The resulting resonance solver allows for efficient gradient-based optimization, demonstrated here by the inverse design of an integrated exciton-polariton cavity. This contribution serves as an important step towards efficient resonance calculations in a variety of multi-scattering scenarios, such as inclusions in stratified media, periodic lattices, and scatterers with arbitrary shapes. A sample refinement strategy suitable for accurately locating a large number of poles is introduced. We tie the AAA algorithm into an automatic differentiation framework to efficiently differentiate multi-scattering resonance calculations. The resulting resonance solver allows for efficient gradient-based optimization, demonstrated here by the inverse design of an integrated exciton-polariton cavity. This contribution serves as an important step towards efficient resonance calculations in a variety of multi-scattering scenarios, such as inclusions in stratified media, periodic lattices, and scatterers with arbitrary shapes.
Lead halide perovskite quantum dots (QDs), the latest generation of the colloidal QD family, exhibit outstanding optical properties, which are now exploited as both classical and quantum light sources. Most of their rather exceptional properties are related to the peculiar exciton fine-structure of band-edge states, which can support unique bright triplet excitons. The degeneracy of the bright triplet excitons is lifted with energetic splitting in the order of millielectronvolts, which can be resolved by the photoluminescence (PL) measurements of single QDs at cryogenic temperatures. Each bright exciton fine-structure-state (FSS) exhibits a dominantly linear polarization, in line with several theoretical models based on the sole crystal field, exchange interaction, and shape anisotropy. Here, we show that in addition to a high degree of linear polarization, the individual exciton FSS can exhibit a non-negligible degree of circular polarization even without external magnetic fields by investigating the four Stokes parameters of the exciton fine-structure in individual CsPbBr3 QDs through Stokes polarimetric measurements. We observe a degree of circular polarization up to ∼38%, which could not be detected by using the conventional polarimetric technique. In addition, we found a consistent transition from left- to right-hand circular polarization within the fine-structure triplet manifold, which was observed in magnetic-field-dependent experiments. Our optical investigation provides deeper insights into the nature of the exciton fine structures and thereby drives the yet-incomplete understanding of the unique photophysical properties of this class of QDs for the benefit of future applications in chiral quantum optics.
Highly ordered nanocrystal (NC) assemblies, namely superlattices (SLs), have been investigated as a building block of novel bright (quantum) light sources because of their unique collective emission process, so-called superfluorescence. Thus far, the primary preparation method for perovskite NC SLs has been drying-mediated self-assembly, in which the NCs spontaneously assemble into SLs while the solvent evaporates. However, this method does not give control over the position and size of assemblies. Hence, it has been challenging to place NC assemblies in photonic device structures. Here, we demonstrate template-assisted self-assembly of CsPbBr3 NCs to achieve precise control of the geometrical features of NC assemblies. A solution of NCs is drop-casted on a substrate with hollow, lithographically-defined template structures made from SiO2. We allow slow solvent evaporation and remove excess NCs from the substrate surface afterward. Thus, NCs only remain in the templates, and the position and size of these NC assemblies can be controlled by changing the design of the hollow structures. We performed time-resolved photoluminescence measurements on these NC assemblies and observed signatures of collective photon emission. Our results provide an important step forward for the development of optical devices that harness embedded perovskite NC assemblies.
The brightness of an emitter is ultimately described by Fermi’s golden rule, with a radiative rate proportional to its oscillator strength times the local density of photonic states. As the oscillator strength is an intrinsic material property, the quest for ever brighter emission has relied on the local density of photonic states engineering, using dielectric or plasmonic resonators 1 , 2 . By contrast, a much less explored avenue is to boost the oscillator strength, and hence the emission rate, using a collective behaviour termed superradiance. Recently, it was proposed 3 that the latter can be realized using the giant oscillator-strength transitions of a weakly confined exciton in a quantum well when its coherent motion extends over many unit cells. Here we demonstrate single-photon superradiance in perovskite quantum dots with a sub-100 picosecond radiative decay time, almost as short as the reported exciton coherence time 4 . The characteristic dependence of radiative rates on the size, composition and temperature of the quantum dot suggests the formation of giant transition dipoles, as confirmed by effective-mass calculations. The results aid in the development of ultrabright, coherent quantum light sources and attest that quantum effects, for example, single-photon emission, persist in nanoparticles ten times larger than the exciton Bohr radius.
Multimode behavior plays a key role in a wide range of nonlinear optical phenomena. Multiple exciton-polariton modes can attain macroscopic population as observed in time-integrated measurements. Recent theory work has shown that, rather than being simultaneously in many modes, the population may temporally switch between the modes. However, the origin and the dynamics of multimode condensation has not been experimentally addressed. Here, we study the dynamics of exciton-polariton condensation into multiple modes of Gaussian defect microcavities filled with ladder type polymer gain material methyl-substituted ladder-type poly(p-phenylene) MeLPPP. We deploy a second-order cumulant model to simulate the dynamics of the system and find picosecond-timescale switching between condensate modes. By interferometric measurements we reveal the experimental signatures of such mode competition behaviour. Recent theoretical works have predicted lasing/condensation in multimode exciton-polaritons, hybrid light-matter quasiparticles, but the origin and the dynamics of multimode condensation has not been experimentally investigated. The authors study the dynamics of multimode exciton-polariton condensation, revealing the experimental signatures of mode competition.
The clock speed of electronic circuits has been stagnant at a few gigahertz for almost two decades because of the breakdown of Dennard scaling, which states that by shrinking the size of transistors they can operate faster while maintaining the same power consumption. Optical computing could overcome this roadblock, but the lack of materials with suitably strong nonlinear interactions needed to realize all-optical switches has, so far, precluded the fabrication of scalable architectures. Recently, microcavities in the strong light-matter interaction regime enabled all-optical transistors which, when used with an embedded organic material, can operate even at room temperature with sub-picosecond switching times, down to the single-photon level. However, the vertical cavity geometry prevents complex circuits with on-chip coupled transistors. Here, by leveraging silicon photonics technology, we show exciton-polariton condensation at ambient conditions in micrometer-sized, fully integrated high-index contrast grating microcavities filled with an optically active polymer. By coupling two resonators and exploiting seeded polariton condensation, we demonstrate ultrafast all-optical transistor action and cascadability. Our experimental findings open the way for scalable, compact all-optical integrated logic circuits that could process optical signals two orders of magnitude faster than their electrical counterparts.
In Bose-Einstein condensates (BEC), spin-orbit coupling (SOC) produces supersolidity. It is a peculiar state of matter, which, in addition to the superfluid behaviour shows periodic density modulation typical for crystals. Here, we report the fabrication of a new type of optical microcavity allowing to achieve room-temperature supersolidity for a quantum fluid of light. The microcavity is filled with a nematic liquid crystal (LC) and two layers of the organic polymer MeLPPP hosting exciton resonances. We demonstrate exciton-polariton condensation in the two distinct degenerate minima of the dispersion created by the LC induced Rashba-Dresselhaus (RD) SOC. The condensate real-space distribution shows density stripes located randomly from one condensate realization to another despite the presence of a random disorder potential. This demonstrates the immunity of stripes against disorder (that is, superfluidity) and the spontaneous breaking of translational invariance. We also report the random appearance of vortices via the Kibble-Zurek mechanism, another smoking gun of superfluidity.
Numerous natural and technological phenomena are governed by resonances. In nanophotonics, resonances often result from the interaction of several optical elements. Controlling these resonances is an excellent opportunity to provide light with properties on demand for applications ranging from sensing to quantum technologies. The inverse design of large, distributed resonators, however, is typically challenged by high computational costs when discretizing the entire system in space. Here, this limitation is overcome by harnessing prior knowledge about the individual scatterers that form the resonator and their interaction. In particular, a transition matrix multi-scattering framework is coupled with the state-of-the-art adaptive Antoulas-Anderson (AAA) algorithm to identify complex poles of the optical response function. A sample refinement strategy suitable for accurately locating a large number of poles is introduced. The AAA algorithm is tied into an automatic differentiation framework to efficiently differentiate multi-scattering resonance calculations. The resulting resonance solver allows for efficient gradient-based optimization, demonstrated here by the inverse design of an integrated exciton-polariton cavity. This contribution serves as an important step towards efficient resonance calculations in a variety of multi-scattering scenarios, such as inclusions in stratified media, periodic lattices, and scatterers with arbitrary shapes.