Exciton-polariton Emission Research Articles

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.

Observation of Room-Temperature Exciton-Polariton Emission from Wide-Ranging 2D Semiconductors Coupled with a Broadband Mie Resonator.

Two-dimensional exciton-polaritons in monolayer transition metal dichalcogenides (TMDs) exhibit practical advantages in valley coherence, optical nonlinearities, and even bosonic condensation owing to their light-emission capability. To achieve robust exciton-polariton emission, strong photon-exciton couplings are required at the TMD monolayer, which is challenging due to its atomic thickness. High-quality (Q) factor optical cavities with narrowband resonances are an effective approach but typically limited to a specific excitonic state of a certain TMD material. Herein, we achieve on-demand exciton-polariton emission from a wide range of TMDs at room temperature by hybridizing excitons with broadband Mie resonances spanning the whole visible spectrum. By confining broadband light at the TMD monolayer, our one type of Mie resonator on different TMDs enables enhanced light-matter interactions with multiple excitonic states simultaneously. We demonstrate multi-Rabi splittings and robust polaritonic photoluminescence in monolayer WSe2, WS2, and MoS2. The hybrid system also shows the potential to approach the ultrastrong coupling regime.

Dynamics of exciton–polariton emission in CuI

We report on temperature-dependent (10 K – 250 K) spectral and dynamical properties of free exciton–polariton and bound exciton emission in copper iodide (CuI) bulk single crystals analyzed by means of time-resolved photoluminescence spectroscopy. The characteristic line shape of the polariton emission at low temperatures is interpreted in terms of the “k-linear term effect” on the degenerate Z1,2 excitons in CuI. For free exciton–polaritons, an increase in the decay time with increasing temperature up to 360 ps at 160 K is observed. For bound exciton emission, decay times between 180 ps and 380 ps are observed at low temperatures, revealing the expected EB3/2 dependence of radiative lifetime on the localization energy. Based on the observed rise times of bound excitons at low temperatures, a defect density of shallow acceptors of 1 × 1017 cm−3 was estimated, in agreement with measured room temperature free hole density.

Plasmon-enhanced strong exciton-polariton coupling in single microwire-based heterojunction light-emitting diodes.

Manipulating the strong light-matter coupling interaction in optical microresonators that are naturally formed by semiconductor micro- or nanostructures is crucial for fabricating high-performance exciton-polariton devices. Such devices can function as coherent light sources having considerably lower emission threshold. In this study, an exciton-polariton light-emitting diode (LED), made of a single ZnO microwire (MW) and a p-GaN substrate, serving as the hole injector, was fabricated, and its working characteristics, in the near-ultraviolet region, were demonstrated. To further improve the quality of the single ZnO MW-based optical microresonator, Ag nanowires (AgNWs) with ultraviolet plasmonic response were deposited on the MW. Apart from the improvement of the electrical and optical properties of the hexagonal ZnO MW, the optically pumped whispering-gallery-mode lasing characteristics were significantly enhanced. Furthermore, a single ZnO MW not covered, and covered by AgNWs, was used to construct a heterojunction LED. Compared with single bare ZnO MW-based LED, significant enhancement of the device performance was achieved, including a significant enhancement in the light output and a small emission band blueshift. Specifically, the exciton-polariton emission was observably enhanced, and the corresponding Rabi splitting energy (∼ 495 meV) was significantly higher than that of the bare ZnO MW-based LED (∼ 370 meV). That ultraviolet plasmons of AgNWs enhanced the exciton-polariton coupling strength was further confirmed via angle-resolved electroluminescence measurements of the single MW-based polaritonic devices, which clearly illustrated the presence of Rabi splitting and subband anti-crossing characteristics. The experimental results provide new avenues to achieve extremely high coupling strengths, which can accelerate the advancements in electrically driven high-efficiency polaritonic coherent emitters and nonlinear devices.

Growth of hopper-shaped CsPbCl3 crystals and their exciton polariton emission.

CsPbCl3 is an attractive wide-bandgap perovskite semiconductor. Herein, we have grown hopper-shaped CsPbCl3 crystals in a solution droplet dripped on a heated substrate. During the growth, we have observed the impacts of the coffee ring effect and Marangoni flow, which may result in the hopper shape. Their photoluminescence spectra feature double peaks, which are located at 413.9 nm and 422.0 nm, respectively, and the latter increases faster in intensity than the former as the excitation power increases. We believe that the higher-energy peak originates from the excitonic emission and the lower-energy one is from the polaritons' emission, where the polaritons are generated in the exciton–exciton inelastic scattering process. Based on such an explanation, the exciton binding energy of CsPbCl3 is estimated to be 76.7 meV in our experiments, consistent with the previous reports.

Spin noise signatures of the self-induced Larmor precession

Bose-Einstein condensates of exciton-polaritons are known for their fascinating coherent and polarization properties. The spin state of the condensate is reflected in polarization of the exciton-polariton emission, with temporal fluctuations of this polarization being, in general, capable of reflecting quantum statistics of polaritons in the condensate. To study the polarization properties of optically trapped polariton condensates, we take advantage of the spin noise spectroscopy technique. The ratio between the noise of ellipticity of the condensate emission and its polarization plane rotation noise is found to be dependent, in a nontrivial way, on the intensity of CW nonresonant laser pumping. We show that the interplay between the ellipticity and the rotation noise can be explained in terms of the competition between the self-induced Larmor precession of the condensate pseudospin and the static polarization anisotropy of the microcavity.

Wavelength-Tunable Waveguide Emissions from Electrically Driven Single ZnO/ZnO:Ga Superlattice Microwires

Because of the superlattice structures comprising periodic and alternating crystalline layers, one-dimensional photon crystals can be employed to expand immense versatility and practicality of modulating the electronic and photonic propagation behaviors, as well as optical properties. In this work, individual superlattice microwires (MWs) comprising ZnO and Ga-doped ZnO (ZnO/ZnO:Ga) layers were successfully synthesized. Wavelength-tunable multipeak emissions can be realized from electrically driven single superlattice MW-based emission devices, with the dominant wavelengths tuned from ultraviolet to visible spectral regions. To illustrate the multipeak character, single superlattice MWs were selected to construct fluorescent emitters, and the emission wavelength could be tuned from 518 to 562 nm, which is dominated by Ga incorporation. Especially, by introducing Au quasiparticle film decoration, emission characteristics can further be modulated, such as the red shift of the emission wavelengths, and the multipeaks were strongly modified and split into more and narrower subbands. In particular, electrically pumped exciton-polariton emission was realized from heterojunction diodes composed of single ZnO/ZnO:Ga superlattice MWs and p-GaN layers in the blue-ultraviolet spectral regions. With the aid of localized surface plasmons from Au nanoparticles, which deposited on the superlattice MW, significant improvement of emission characteristics, such as enhancement of output efficiencies, blue shift of the dominant emission wavelengths, and narrowing of the spectral linewidth, can be achieved. The multipeak emission characteristics would be originated from the typical optical cavity modes, but not the Fabry-Perot mode optical cavity formed by the bilateral sides of the wire. The resonant modes are likely attributed to the coupled optical microcavities, which formed along the axial direction of the wire; thus, the emitted photons can be propagated and selected longitudinally. Therefore, the novel ZnO/ZnO:Ga superlattice MWs with a quadrilateral cross section can provide a potential platform to construct multicolor emitters and low-threshold exciton-polariton diodes and lasers.

Elliptically polarized exciton-polariton condensate in a semiconductor microcavity with a chiral photonic crystal slab

We demonstrate a method for controling polarization of exciton-polariton condensate emission in a planar semiconductor microcavity based on modification of the electromagnetic mode structure in the microcavity. The modification is realized by fabrication of a chiral photonic crystal slab with partial etching of the upper Bragg mirror lowering the microcavity symmetry to C4. A degree of circular polarization as high as 70% has been demonstrated experimentally in the structure with optimized parameters without the use of a static magnetic field or birefringent wave plates.

Near-infrared exciton-polaritons in strongly coupled single-walled carbon nanotube microcavities.

Exciton-polaritons form upon strong coupling between electronic excitations of a material and photonic states of a surrounding microcavity. In organic semiconductors the special nature of excited states leads to particularly strong coupling and facilitates condensation of exciton-polaritons at room temperature, which may lead to electrically pumped organic polariton lasers. However, charge carrier mobility and photo-stability in currently used materials is limited and exciton-polariton emission so far has been restricted to visible wavelengths. Here, we demonstrate strong light-matter coupling in the near infrared using single-walled carbon nanotubes (SWCNTs) in a polymer matrix and a planar metal-clad cavity. By exploiting the exceptional oscillator strength and sharp excitonic transition of (6,5) SWCNTs, we achieve large Rabi splitting (>110 meV), efficient polariton relaxation and narrow band emission (<15 meV). Given their high charge carrier mobility and excellent photostability, SWCNTs represent a promising new avenue towards practical exciton-polariton devices operating at telecommunication wavelengths.

Room-Temperature Observation of Trapped Exciton-Polariton Emission in GaN/AlGaN Microcavities with Air-Gap/III-Nitride Distributed Bragg Reflectors

We demonstrate trapped exciton-polariton emission at room temperature from nonpolar GaN/AlGaN cavities sandwiched between air/AlGaN distributed Bragg reflectors. Nanoscale thickness fluctuations characteristic to the nonpolar AlGaN cavity layer create deep potential traps, giving rise to a strong (in-plane) localization of exciton-polaritons. The observed quantized exciton-polariton states exhibit a large quantized energy of up to 6 meV, which benefits from the wide bandgap of III-nitrides. The experimental results are well explained by numerical simulations. III-Nitride exciton-polaritons in such deep traps will be useful for practical exciton-polariton lasers with high degrees of coherence and high-repetition rate Josephson oscillators with multicomponent condensates.

Spin noise of a polariton laser

We report on experimental study of the exciton-polariton emission (PE) polarization noise below and above the polariton lasing threshold under continuous wave nonresonant excitation. The experiments were performed with a high-Q graded 5{\lambda}/2 GaAs/AlGaAs microcavity with three quantum wells in the strong coupling regime. The PE polarization noise substantially exceeded in magnitude the shot noise level and, in the studied frequency range (up to 650 MHz), had a flat spectrum. We have found that the PE polarization noise magnitude dependence on the pump intensity showed specific features that had no analogy in power dependences of the PE intensity and intensity noise. Particularly, the linear polarization fluctuations normalized by the emission intensity showed a remarkably non-monotonic dependence on the pump power. A theoretical model describing the observed peculiarity of the PE polarization noise is proposed.

Directional exciton-polariton photoluminescence emission from terminals of a microsphere-coupled organic waveguide

We report on angle-resolved, exciton-polariton photoluminescence measurements from asymmetric terminals of a microsphere-coupled organic waveguide (MOW). The MOW architecture consisted of a SiO2 microsphere coupled with a diaminoanthroquinone mesowire, self-assembled on a glass substrate. The angle-resolved emission measurements were performed using spatially filtered Fourier-plane optical imaging method. The light emanating from the sphere-terminus had two regions of angular emission in the Fourier-plane, of which one had azimuthal angular spread as small as 10°. The emission from wire terminus was uni-directional in nature, with some light emitted beyond the critical angle of glass-air interface. Our results highlight unique directional emission characteristics of a hybrid organic waveguide geometry and may have implications on single-element, exciton-polariton based light-emitting devices and lasers.

Plasmon-controlled excitonic emission from vertically-tapered organic nanowires.

Organic molecular nanophotonics has emerged as an important avenue to harness molecular aggregation and crystallization on various functional platforms to obtain nano-optical devices. To this end, there is growing interest to combine organic molecular nanostructures with plasmonic surfaces and interfaces. Motivated by this, herein we introduce a unique geometry: vertically-tapered organic nanowires grown on a plasmonic thin film. A polarization-sensitive plasmon-polariton on a gold thin-film was harnessed to control the exciton-polariton propagation and subsequent photoluminescence from an organic nanowire made of diaminoanthraquinone (DAAQ) molecules. We show that the exciton-polariton emission from individual DAAQ nanowires can be modulated up to a factor of 6 by varying the excitation polarization state of surface plasmons. Our observations were corroborated with full-wave three-dimensional finite-difference time-domain calculations performed on vertically-tapered nanowire geometry. Our work introduces a new optical platform to study coupling between propagating plasmons and propagating excitons, and may have implications in emerging fields such as hybrid-polariton based light emitting devices and vertical-cavity nano-optomechanics.

F-band condensates in exciton-polariton lattice systems

We report the condensation of microcavity exciton-polaritons at $\ensuremath{\Gamma}$ points located on the boundary between the third and higher Brillouin zones in hexagonal lattices: triangular and honeycomb geometries. We collect experimental evidence that supports the finite momentum condensation: (1) the coherent Bragg peaks formed at nonzero $\ensuremath{\Gamma}$ points; (2) the nonlinear intensity increase in the exciton-polariton emission at quantum degeneracy threshold; (3) the spectral linewidth behavior: narrowing near threshold and broadening above threshold; and (4) the equivalent 4${f}_{{y}^{3}\ensuremath{-}3{x}^{2}y}$-like orbital symmetry in real space. The $f$-orbital state at $\ensuremath{\Gamma}$ points appears as a metastable momentum valley to trap exciton-polaritons, which is explained by single-particle band-structure calculations.

Vacuum Rabi Splitting of Exciton–Polariton Emission in an AlN Film

The vacuum Rabi splitting of exciton–polariton emission is observed in cathodoluminescence (CL) and photoluminescence spectra of an AlN epitaxial film. Atomic force microscopy and CL measurements show that the film has an atomically flat surface, high purity, and high crystal quality. By changing the temperature, anticrossing behavior between the upper and lower polariton branch can be obtained in low temperature with a Rabi splitting of 44 meV, in agreement with the calculation. This large energy splitting is caused by strong oscillator strength, intrinsically pure polarization in wurtzite AlN semiconductor, and high fraction of free exciton in the sample. These properties indicate that AlN can be a potential semiconductor for the further development of polariton physics and polariton–based novel devices.

Room Temperature Current Injection Polariton Light Emitting Diode with a Hybrid Microcavity

The strong light-matter interaction within a semiconductor high-Q microcavity has been used to produce half-matter/half-light quasiparticles, exciton-polaritons. The exciton-polaritons have very small effective mass and controllable energy-momentum dispersion relation. These unique properties of polaritons provide the possibility to investigate the fundamental physics including solid-state cavity quantum electrodynamics, and dynamical Bose-Einstein condensates (BECs). Thus far the polariton BEC has been demonstrated using optical excitation. However, from a practical viewpoint, the current injection polariton devices operating at room temperature would be most desirable. Here we report the first realization of a current injection microcavity GaN exciton-polariton light emitting diode (LED) operating under room temperature. The exciton-polariton emission from the LED at photon energy 3.02 eV under strong coupling condition is confirmed through temperature-dependent and angle-resolved electroluminescence spectra.

Exciton-polariton microphotoluminescence and lasing from ZnO whispering-gallery mode microcavities

Hexagonal ZnO microrods were employed as whispering-gallery mode (WGM) optical microcavities to investigate exciton-polariton microphotoluminescence and lasing emission. Using a confocal microphotoluminescence system, the exciton-polariton emission with a large Rabi splitting of about 90 meV was observed from a ZnO microrod with the diameter of 9.38 μm. The spatial-resolved spectra demonstrated a collective nonlinear blueshift in the WGM resonance peaks along a tapered microrod and proved the anticross dispersion property of the exciton-polariton. Furthermore, the exciton-polariton WGM lasing was stimulated and blueshifted in the strong coupling region under the excitation of a 355 nm nanosecond pulsed laser.

Enhanced exciton photoluminescence in the selectively Si-doped GaAs/AlxGa1−xAs heterostructures

Experimental results examining the photoluminescence spectra of selectively Si-doped GaAs/AlxGa1−xAs heterostructures is presented. Possible mechanisms of carrier recombination are discussed with a special emphasis on the peculiarities of excitonic photoluminescence. Strong intensity lines in photoluminescence spectra are associated with the formation and enhancement of free exciton and exciton-polariton emission in the flat band region of an active i-GaAs layer. The excitonic PL intensity is sensitive to the excitation intensity indicating high nonlinear behavior of spectral-integrated photoluminescence intensity and exciton line narrowing. These observed phenomena may be related to the collective interaction of excitons and the interaction of excitons with emitted electromagnetic waves. The gain of the amplification of the excitonic photoluminescence intensity in the heterostructure was found to be more than 1000 times larger than the intensity of i-GaAs active layer. The quality factor of the exciton line emission and the exciton-polariton line was found to be 3800 and 7600, respectively.

Unique photoluminescence from ZnO grown by eclipse pulsed laser deposition

Nanostructured ZnO was deposited by eclipse pulsed laser deposition from a metallic Zn target in an oxygen atmosphere. Photoluminescence (PL) was carried out on the structures at liquid helium temperatures. The temperature dependence of the PL as well as the power dependence at 4 K gave insight into the processes governing the light emission from these samples. Free A and B excitonic emission was observed as well as exciton-polariton emission from the upper and lower polariton branches. The low temperature PL was dominated by the I7 exciton, which currently has an unknown chemical origin and is not commonly observed in the PL spectrum of bulk ZnO. Power dependence of the I7 feature showed unique behavior not previously reported. All the other features had nearly linear power dependence while the I7 peak had an emission exponent of 1.53±0.01. Lead was the dominant impurity in the Zn target used to grow the eclipse pulsed laser deposited (EPLD) samples and seemed a likely candidate for the origin of the I7 excitonic peak. Implantation of Pb into bulk ZnO showed no appearance of the I7 feature at 0.01% Pb concentration. As such, Pb may not be the origin of the I7 feature which dominates the PL from the EPLD grown samples. However, due to the complicated interactions of Pb in a ZnO host, it is likely that the Pb is incorporated differently in the implanted bulk and EPLD grown ZnO.

Polarization behavior of the exciton-polariton emission of ZnO-based microresonators

AbstractWe present the polarization behavior of the exciton-polariton luminescence of a ZnO-based all-oxide resonator. A splitting in the emission energy between the s- and p-polarized pho-toluminescence of the lower polariton branch was observed which increases with increasing emission angle. It is caused by the polarization behavior of the uncoupled cavity-photon mode, and reaches a maximum of about 5 meV at an emission angle near the bottleneck region. For lar-ger angles the energy splitting decreases. Additionally to the energy splitting, we observed dif-ferences in the photoluminescence intensity which we trace back to different occupation of the lower polariton branch for the two polarizations. Whereas for p-polarization a bottleneck effect is clearly observable, this effect is much weaker for s-polarization. These findings indicate that the relaxation of hot carriers into the bottleneck region is enhanced for the p-polarized photolumi-nescence compared to the s-polarized one. The differences between these two polarizations are most pronounced for a very large negative detuning and vanish with increasing detuning.