Polariton Lasing Research Articles

Circumventing the polariton bottleneck via dark excitons in 2D semiconductors

Efficient scattering into the exciton polariton ground state is a key prerequisite for generating Bose–Einstein condensates and low-threshold polariton lasing. However, this can be challenging to achieve at low densities due to the polariton bottleneck effect that impedes phonon-driven scattering into low-momentum polariton states. The rich exciton landscape of transition metal dichalcogenides (TMDs) provides potential intervalley scattering pathways via dark excitons to rapidly populate these polaritons. Here, we present a theoretical and fully microscopic study exploring the time- and momentum-resolved relaxation of exciton polaritons supported by a MoSe2 monolayer integrated within a Fabry–Perot cavity. By exploiting phonon-assisted transitions between momentum-dark excitons and the lower polariton branch, we demonstrate that it is possible to circumvent the bottleneck region and efficiently populate the polariton ground state. Furthermore, this intervalley pathway is predicted to give rise to, yet unobserved, angle-resolved phonon sidebands in low-temperature photoluminescence spectra that are associated with momentum-dark excitons. This represents a distinct signature for efficient phonon-mediated polariton-dark-exciton interactions.

Organic polaritonic light-emitting diodes with high luminance and color purity toward laser displays

Achieving high-luminescence organic light-emitting devices (OLEDs) with narrowband emission and high color purity is important in various optoelectronic fields. Laser displays exhibit outstanding advantages in next-generation display technologies owing to their ultimate visual experience, but this remains a great challenge. Here, we develop a novel OLED based organic single crystals. By strongly coupling the organic exciton state to an optical microcavity, we obtain polariton electroluminescent (EL) emission from the polariton OLEDs (OPLEDs) with high luminance, narrow-band emission, high color purity, high polarization as well as excellent optically pumped polariton laser. Further, we evaluate the potential for electrically pumped polariton laser through theoretical analysis and provide possible solutions. This work provides a powerful strategy with a material–device combination that paves the way for electrically driven organic single-crystal-based polariton luminescent devices and possibly lasers.

Dark State Concentration Dependent Emission and Dynamics of CdSe Nanoplatelet Exciton-Polaritons.

The recent surge of interest in polaritons has prompted fundamental questions about the role of dark states in strong light-matter coupling phenomena. Here, we systematically vary the relative number of dark states by controlling the number of stacked CdSe nanoplatelets confined in a Fabry-Pérot cavity. We find the emission spectrum to change significantly with an increasing number of nanoplatelets, with a gradual shift of the dominant emission intensity from the lower polariton branch to a manifold of dark states. Through accompanying calculations based on a kinetic model, this shift is rationalized by an entropic trapping of excitations by the dark state manifold, while a weak dark state dispersion due to local disorder explains their nonzero emission. Our results point toward the relevance of the dark state concentration to the optical and dynamical properties of cavity-embedded quantum emitters with ramifications for Bose-Einstein condensate formation, polariton lasing, polariton-based quantum transduction schemes, and polariton chemistry.

Ultra-thin size-controllable surface plasmon polariton laser by PDMS-assisted imprinting

Plasmonic laser has great potential to overcome the optical diffraction limit, playing a crucial role in advancing nanophotonics and nanoelectronics for on-chip integration. However, current plasmonic lasers face several challenges, such as the difficulty in controlling nanowire (NW) size, disordered arrangement, and complicated fabrication process. Herein, ultra-thin gain media for plasmonic lasers below the cutoff size of the photonic mode are prepared using the polydimethylsiloxane-assisted imprinting. This method enables precise control over the size of the perovskite NW, with the minimum size achievable being 60 nm. As a result, the plasmonic lasing is achieved from the CsPbBr3 NW-based device with a threshold as low as ∼49.13 μJ cm−2 and a Quality Factor (Q) of 1803 at room temperature, demonstrating its capability for achieving high-quality lasing. Meanwhile, a dual-pumping time-resolved fluorescence study suggests that the radiative recombination lifetime of CsPbBr3 NWs is shortened by a factor of 10 due to the Purcell effect, confirming the plasmonic effect exhibited by the device. Furthermore, a plasmonic laser array is developed using this method, demonstrating the applicability of the imprinting method in complex graphic fabrication. This breakthrough provides a solution for the application of plasmonic laser arrays in optoelectronic integration.

A near-resonant excitation strategy to achieve ultra-low threshold GaN polariton lasing.

A near-resonant excitation strategy is proposed and implemented in a 4-µm-thick GaN microcavity to realize an exciton-polariton condensate/lasing with low threshold. Strong exciton-photon coupling is demonstrated, and polariton lasing is realized with an ultra-low threshold excitation power density of about 13.3 W/cm2 at room temperature. Such an ultra-low threshold is ascribed to the implementation of the near-resonant optical excitation strategy, which enables acceleration of the exciton and polariton relaxation and suppression of the heat generation in the cavity, thereby reducing the energy loss and enhance the cavity excitation efficiency.

Quantized Microcavity Polariton Lasing Based on InGaN Localized Excitons.

Exciton-polaritons, which are bosonic quasiparticles with an extremely low mass, play a key role in understanding macroscopic quantum effects related to Bose-Einstein condensation (BEC) in solid-state systems. The study of trapped polaritons in a potential well provides an ideal platform for manipulating polariton condensates, enabling polariton lasing with specific formation in k-space. Here, we realize quantized microcavity polariton lasing in simple harmonic oscillator (SHO) states based on spatial localized excitons in InGaN/GaN quantum wells (QWs). Benefiting from the high exciton binding energy (90 meV) and large oscillator strength of the localized exciton, room-temperature (RT) polaritons with large Rabi splitting (61 meV) are obtained in a strongly coupled microcavity. The manipulation of polariton condensates is performed through a parabolic potential well created by optical pump control. Under the confinement situation, trapped polaritons are controlled to be distributed in the selected quantized energy sublevels of the SHO state. The maximum energy spacing of 11.3 meV is observed in the SHO sublevels, indicating the robust polariton trapping of the parabolic potential well. Coherent quantized polariton lasing is achieved in the ground state of the SHO state and the coherence property of the lasing is analyzed through the measurements of spatial interference patterns and g(2)(τ). Our results offer a feasible route to explore the manipulation of macroscopic quantum coherent states and to fabricate novel polariton devices towards room-temperature operations.

Mode-locked waveguide polariton laser

So far, exciton-polariton (polariton) lasers were mostly single-mode lasers based on microcavities. Despite the large repulsive polariton-polariton interaction, a pulsed mode-locked polariton laser was never, to our knowledge, reported. Here, we use a 60-µm-long GaN-based waveguide surrounded by distributed Bragg reflectors forming a multi-mode horizontal cavity. We demonstrate experimentally and theoretically a polariton mode-locked micro-laser operating in the blue-UV, at room temperature, with a 300 GHz repetition rate and 100-fs-long pulses. The mode-locking is demonstrated by the compensation (linearization) of the mode dispersion by the self-phase modulation induced by the polariton-polariton interaction. It is also supported by the observation in experiment and theory of the typical envelope frequency profile of a bright soliton.

Ultrafast Dynamics of Bloch Surface Wave Polaritons in Large-Area 2D Semiconductor Monolayers at Room Temperature.

The dynamics of strongly coupled polariton systems integrated with 2D transition metal dichalcogenides (TMDs) is key to enabling efficient coherent processes and achieving high-performance TMD-based polaritonic devices, such as ultralow-threshold polariton lasers and ultrafast optical switches. However, there has been a lack of a comprehensive understanding of the excited state dynamics in TMD-based polariton systems. In this work, ultrafast pump-probe optical spectroscopy is used to investigate the room temperature dynamics of the polariton systems consisting of TMD monolayer excitons strongly coupled with Bloch surface waves (BSWs) supported by all-dielectric photonic structures. The transient response is found for both above-exciton energy pumping and polariton-resonant pumping. The excited state population and ultrafast coherent coupling of the exciton reservoir and lower polariton (LP) branch are observed for resonant pumping. Moreover, it is found that the transient response of the LP first decays on a short-time scale of 0.15-0.25ps compared to the calculated intrinsic lifetime of 0.11-0.20ps, and is followed by a longer decay (>100ps) due to the dynamical evolution of the exciton reservoir. The results provide a fundamental understanding of the dynamics of TMD-based polariton systems while showing the potential for achieving efficient coherent optical processes for device applications.

High Efficiency of Exciton-Polariton Lasing in a 2D Multilayer Structure.

We have placed a van der Waals homostructure, formed by stacking three two-dimensional layers of WS2 separated by insulating hBN, similar to a multiple-quantum well structure, inside a microcavity, which facilitates the formation of quasiparticles known as exciton-polaritons. The polaritons are a combination of light and matter, allowing laser emission to be enhanced by nonlinear scattering, as seen in prior polariton lasers. In the experiments reported here, we have observed laser emission with an ultralow threshold. The threshold was approximately 59 nW/μm2, with a lasing efficiency of 3.82%. These findings suggest a potential for efficient laser operations using such homostructures.

Room-Temperature Polariton Lasing from CdSe Core-Only Nanoplatelets.

This paper reports how CdSe core-only nanoplatelets (NPLs) coupled with plasmonic Al nanoparticle lattices can exhibit exciton-polariton lasing. By improving a procedure to synthesize monodisperse 4-monolayer CdSe NPLs, we could resolve polariton decay dynamics and pathways. Experiment and theory confirmed that the system is in the strong coupling regime based on anticrossings in the dispersion diagrams and magnitude of the Rabi-splitting values. Notably, polariton lasing is observed only for cavity lattice periodicities that exhibit specific dispersive characteristics that enable polariton accumulation. The threshold of polariton lasing is 25-fold lower than the reported photon lasing values from CdSe NPLs in similar cavity designs. This open-cavity platform offers a simple approach to control exciton polaritons anticipated to benefit quantum information processing, optoelectronics, and chemical reactions.

Ultra‐Narrow Linewidth Polariton Lasing in Optically Trapped Bose‐Einstein Condensates at Room Temperature

AbstractPolariton lasing via Bose‐Einstein condensation (BEC) provides a peculiar method to achieve low threshold coherent light sources. Until now, the cryogenic operating temperature required for polariton lasers has hampered the development of polaritonics. Here, a novel approach is first reported to realize the ultra‐narrow linewidth polariton lasing under quasi‐3D quantum confinement at room‐temperature (RT). The potential trap landscape is constructed by ring‐shaped optical excitation, wherein the continuum polariton dispersion is modulated into discrete simple harmonic oscillator (SHO) states. The coherent condensation lasing of trapped polaritons occurs beyond the threshold power. Benefiting from the horizontal quantum confinement, the trapped polariton lasing exhibits an ultra‐narrow linewidth (0.7 meV) and excellent quality factor (Q = 3510). Moreover, the second‐order quantum coherence properties of trapped polariton condensation are determined to reveal the quantum phase transition of Bosonic system. The results offer a feasible route for realizing a low‐threshold ultra‐narrow linewidth polariton laser at RT, which significantly facilitates the fabrication of polariton laser and switches on opportunities for future applications.

An Electrically Pumped Topological Polariton Laser.

With a seminal work of Raghu and Haldane in 2008, concepts of topology have been introduced into optical systems, where some of the most promising routes to an application are efficient and highly coherent topological lasers. While some attempts have been made to excite such structures electrically, the majority of published experiments use a form of laser excitation. In this paper, we use a lattice of vertical resonator polariton micropillars to form an exponentially localized topological Su-Schrieffer-Heeger defect. Upon electrical excitation, the system unequivocally shows polariton lasing from the topological defect using a carefully placed gold contact. Despite the presence of doping and electrical contacts, the polariton band structure clearly preserves its topological properties. At high excitation power the Mott density is exceeded, leading to highly efficient lasing in the weak coupling regime. This work is an important step toward applied topological lasers using vertical resonator microcavity structures.

Dirac Cones and Room Temperature Polariton Lasing Evidenced in an Organic Honeycomb Lattice.

Artificial 1D and 2D lattices have emerged as a powerful platform for the emulation of lattice Hamiltonians, the fundamental study of collective many-body effects, and phenomena arising from non-trivial topology. Exciton-polaritons, bosonic part-light and part-matter quasiparticles, combine pronounced nonlinearities with the possibility of on-chip implementation. In this context, organic semiconductors embedded in microcavities have proven to be versatile candidates to study nonlinear many-body physics and bosonic condensation, and in contrast to most inorganic systems, they allow the use at ambient conditions since they host ultra-stable Frenkel excitons. A well-controlled, high-quality optical lattice is implemented that accommodates light-matter quasiparticles. The realized polariton graphene presents with excellent cavity quality factors, showing distinct signatures of Dirac cone and flatband dispersions as well as polariton lasing at room temperature. This is realized by filling coupled dielectric microcavities with the fluorescent protein mCherry. The emergence of a coherent polariton condensate at ambient conditions are demonstrated, taking advantage of coupling conditions as precise and controllable as in state-of-the-art inorganic semiconductor-based systems, without the limitations of e.g. lattice matching in epitaxial growth. This progress allows straightforward extension to more complex systems, such as the study of topological phenomena in 2D lattices including topological lasers and non-Hermitian optics.

Whispering-Gallery Quantum-Well Exciton Polaritons in an Indium Gallium Arsenide Microdisk Cavity.

Despite appealing high-symmetry properties that enable strong spatial confinement and ultrahigh-Q, optical whispering-gallery modes of spherical and circular resonators have been absent from the field of quantum-well exciton polaritons. Here we observe whispering-gallery exciton polaritons in a gallium arsenide microdisk cavity filled with indium gallium arsenide quantum wells, the test bed materials of polaritonics. Strong coupling is evidenced in photoluminescence and resonant spectroscopy accessed through concomitant confocal microscopy and near-field optical techniques. Excitonic and optical resonances are tuned by varying temperature and disk radius, revealing Rabi splittings between 5 and 10meV. A dedicated analytical quantum model for such circular whispering-gallery polaritons is developed, which reproduces the measured values. At high power, lasing is observed and accompanied by a blueshift of the emission consistent with the regime of polariton lasing. With experimental methods and theory now established, whispering-gallery-mode polaritons in round dielectric resonators appear as a new viable platform toward low loss polaritonics.

A highly stable and efficient organic microcavity polariton laser

With their remarkably low thresholds, organic polariton lasers are a promising alternative to organic photonic lasers. However, device stability remains a challenge, in part due to material degradation during deposition of the top dielectric mirror. We demonstrate polariton lasers based on 4,4′-Bis(4-(9H-carbazol-9-yl)styryl)biphenyl (BSBCz) as active material that achieve a low lasing threshold of 8.7 μJ/cm2, and we show that a ZrO2 protection layer between active layer and top mirror significantly improves stability. Optimized devices exhibit minimal degradation after 100,000 excitation pulses at 3.8 times above threshold. Our findings establish BSBCz as an attractive candidate for future injection driven polariton lasers.Graphical abstract

Electrical polarization switching of perovskite polariton laser

Abstract Optoelectronic and spinoptronic technologies benefit from flexible and tunable coherent light sources combining the best properties of nano- and material-engineering to achieve favorable properties such as chiral lasing and low threshold nonlinearities. In this work we demonstrate an electrically wavelength- and polarization-tunable room temperature polariton laser due to emerging photonic spin–orbit coupling. For this purpose, we design an optical cavity filled with both birefringent nematic liquid crystal and an inorganic perovskite. Our versatile growth method of single CsPbBr3 inorganic perovskite crystals in polymer templates allows us to reach strong light–matter coupling and pump-induced condensation of exciton–polaritons resulting in coherent emission of light. The sensitivity of the liquid crystal to external voltage permits electrical tuning of the condensate energy across 7 nm; its threshold power, allowing us to electrically switch it on and off; and its state of polarization sweeping from linear to locally tilted circularly polarized emission.

Investigation of intracavity MgO:LiNbO3 terahertz polariton laser gain over an extended 1–5 THz range

Most intracavity MgO:LiNbO3 terahertz polariton lasers generate output in the 1–3 THz range. In this study, we investigate the potential to extend this tuning range toward 6 THz. We predict broader tuning using a modified polariton gain theory that takes account of additional polariton damping at 3.15 THz and the angle-dependent field overlap in the crystal. We achieved continuous tuning between 1.5 and 5.4 THz and characterised the gain in this range—so far the widest THz frequency range achieved from a nonlinear crystal via intracavity SPS.

Plasmonically-boosted exciton-photon coupling strength in a near-infrared LED based on a ZnO:Ga microwire/GaAs heterojunction with surface-coated Au&Ag alloy nanorods.

The development of electrically-driven low-dimensional coherent light sources via highly-polarized polariton emission behavior has been extensively researched, but suffers from limited modulation of the exciton-photon coupling strengths. Herein, an electrically-biased near-infrared exciton-polariton light-emitting diode (LED), which includes a Ga-doped ZnO microwire (ZnO:Ga MW) and p-type GaAs substrate, is demonstrated. The well-designed LED structure is conducive to producing strong coupling between excitons and cavity photons, thus yielding highly-polarized light-emissions due to the optical birefringence in the ZnO:Ga MW microcavity. In particular, when the LED device is modified using Au&Ag alloy nanorods (AuAgNRs) with desired plasmonic properties, the electroluminescence (EL) performance is significantly boosted, especially the Rabi-splitting energy, which increases from 96 to 285 meV. The current-injection exciton-polariton emission from the LED undergoing a strong coupling regime is confirmed through angle-resolved EL measurements. This study exhibits a performance-boosted near-infrared exciton-polariton LED at room temperature, which provides a new scheme toward the realization of highly energy-efficient polariton coherent light sources. Further, the significantly lower density of polariton states induced by the incorporated metal nanostructures highlights a bright future of realizing ultralow-threshold polariton lasers much more feasibly, in comparison to conventional lasers based on narrow bandgap semiconductors.

Advancements in nanoscale coherent emitters: The development of substrate-free surface plasmon nanolasers

The surface plasmon effect can be used to confine electromagnetic fields to a small footprint measuring tens of nanometers. The resultant resonant cavities function as optimal coherent light sources with subwavelength scale configurations. The plasmonic laser sources based on nanoshell structures, in particular, have demonstrated the potential for use in the detection of subcellular mesoscopic molecular structures. However, this structure has a high plasmon dephasing rate, which can increase the threshold of the device, making it difficult to achieve electrically excited structures, thereby rendering them unsuitable as an active component for integration into optoelectronic circuits. A different approach to confining electromagnetic fields involves using a propagating surface plasmon laser structured on a planar layered semiconductor–insulator–metal. This design enables the surface plasmon to propagate along the direction of the nanowire and offers the potential to achieve electrically driven structures by injecting current into the semiconductor nanowire. Consequently, this structure is more effective in guiding energy into integrated optoelectronic circuits compared to the isotropic radiation of nanoshell structures. However, this design also necessitates a supporting substrate, resulting in the actual device volume exceeding the nanoscale and, in some cases, even larger than the size of a cell. This limitation hinders the application of integrated optoelectronic circuits at the micro/nanoscale for bio-applications. To address these challenges, we developed a substrate-free surface plasmon polariton laser. We demonstrated that allowing direct contact between the film and the air significantly reduced the laser threshold. Furthermore, the device maintained its operational capability across different surfaces.

Anapole assisted self-hybridized exciton-polaritons in perovskite metasurfaces.

The exciton-polaritons in a lead halide perovskite not only have great significance for macroscopic quantum effects but also possess vital potential for applications in ultralow-threshold polariton lasers, integrated photonics, slow-light devices, and quantum light sources. In this study, we have successfully demonstrated strong coupling with huge Rabi splitting of 553 meV between perovskite excitons and anapole modes in the perovskite metasurface at room temperature. This outcome is achieved by introducing anapole modes to suppress radiative losses, thereby confining light to the perovskite metasurface and subsequently hybridizing it with excitons in the same material. Our results indicate the formation of self-hybridized exciton-polaritons within the perovskite metasurface, which may pave the way towards achieving high coupling strengths that could potentially bring exciting phenomena to fruition, such as Bose-Einstein condensation as well as enabling applications such as efficient light-emitting diodes and lasers.