RESUMEN
Exciton polaritons have shown great potential for applications such as low-threshold lasing, quantum simulation, and dissipation-free circuits. In this paper, we realize a room temperature ultrafast polaritonic switch where the Bose-Einstein condensate population can be depleted at the hundred femtosecond timescale with high extinction ratios. This is achieved by applying an ultrashort optical control pulse, inducing parametric scattering within the photon part of the polariton condensate via a four-wave mixing process. Using a femtosecond angle-resolved spectroscopic imaging technique, the erasure and revival of the polariton condensates can be visualized. The condensate depletion and revival are well modeled by an open-dissipative Gross-Pitaevskii equation including parametric scattering process. This pushes the speed frontier of all-optical controlled polaritonic switches at room temperature towards the THz regime.
RESUMEN
Based on ZnO microcavities with high quality factors, where the gain medium exhibits confinement of wave packets due to the intrinsically formed whispering gallery microcavity, strong coupling between excitons and cavity photons can be obtained at room temperature resulting in hybrid quasiparticles, e.g. exciton polaritons. In this work, polariton condensation is induced under the non-resonant excitation by linearly polarized femtosecond laser pulses with different polarization directions. The dynamical angle-resolvedk-space spectra of the photoluminescence emission of polariton condensates are measured with sub-picosecond resolution by the self-developed femtosecond angle-resolved spectroscopic imaging technique. Our results show that the ultrafast dynamics of polariton condensation is sensitive to the polarization direction of the excitation pulses which can be explained qualitatively by the combined effect of selective excitation of distinct exciton modes in the sample and the effective coupling strength of the excitation pulses in the ZnO microcavity for various polarization directions. This work strengthened the understanding of the condensation process for cavity exciton polaritons at room temperature.
RESUMEN
Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. Here, by using a femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity are explicitly visualized. Clear ladder-form build-up processes from higher to lower energy branches of the polariton condensates are observed, which are well reproduced by modeling using rate equations. Remarkably, a pronounced superbunching feature, which could serve as solid evidence for bosonic cascades, is demonstrated by the measured second-order time correlation factor. In addition, the nonlinear polariton parametric scattering dynamics on a time scale of hundreds of femtoseconds are revealed. Our understandings pave the way toward ultrafast coherent control of polaritons at room temperature.
RESUMEN
In this work, by using femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of confined exciton-polaritons in an optical induced potential well based on a ZnO whispering-gallery microcavity is explicitly visualized. The sub-picosecond transition between succeeding quantum harmonic oscillator states can be experimentally distinguished. The landscape of the potential well can be modified by the pump power, the spatial distance and the time delay of the two input laser pulses. Clarifying the underlying mechanism of the polariton harmonic oscillator is interesting for the applications of polariton-based optoelectronic devices and quantum information processing.
RESUMEN
Lead-halide perovskites are generally excellent light emitters and can have larger exciton binding energies than thermal energy at room temperature, exhibiting great promise for room-temperature exciton-polaritonics. Rapid progress has been made recently, although challenges and mysteries remain in lead-halide perovskite semiconductors to push polaritons to room-temperature operation. In this Perspective, we discuss fundamental aspects of perovskite semiconductors for exciton-polaritons and review the recent rapid experimental advances using lead-halide perovskites for room-temperature polaritonics, including the experimental realization of strong light-matter interaction using various types of microcavities as well as reaching the polariton condensation regime in planar microcavities and lattices.
RESUMEN
Distinct from carbon nanotubes, transition-metal dichalcogenide (TMD) nanotubes are noncentrosymmetric and polar and can exhibit some intriguing phenomena such as nonreciprocal superconductivity, chiral shift current, bulk photovoltaic effect, and exciton-polaritons. However, basic characterizations of individual TMD nanotubes are still quite limited, and much remains unclear about their structural chirality and electronic properties. Here we report an optical second-harmonic generation (SHG) study on multiwalled WS2 nanotubes on a single-tube level. As it is highly sensitive to the crystallographic symmetry, SHG microscopy unveiled multiple structural domains within a single WS2 nanotube, which are otherwise hidden under conventional white-light optical microscopy. Moreover, the polarization-resolved SHG anisotropy patterns revealed that different domains on the same tube can be of different chirality. In addition, we observed the excitonic states of individual WS2 nanotubes via SHG excitation spectroscopy, which were otherwise difficult to acquire due to the indirect band gap of the material.
RESUMEN
Macroscopic coherence of Bose condensates is a fundamental and practical phenomenon in many-body systems, such as the long-range correlation of exciton-polariton condensates with a dipole density typically below the exciton Mott-transition limit. Here we extend the macroscopic coherence of electron-hole-photon interacting systems to a new region in the phase diagram-the high-density plasma region, where long-range correlation is generally assumed to be broken due to the rapid dephasing. Nonetheless, a cooperative state of electron-hole plasma does emerge through the sharing of the superfluorescence field in an optical microcavity. In addition to the in situ coherence of e-h plasma, a long-range correlation is formed between two 8-µm-spaced plasma ensembles even at room temperature. Quantized and self-modulated correlation modes are generated for e-h ensembles in the plasma region. By controlling the distance between the two ensembles, multiple coupling regimes are revealed, from strong correlation to perturbative phase correlation and finally to an incoherent classical case, which has potential implications for tunable and high-temperature-compatible quantum devices.
RESUMEN
Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2-7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8-11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry-and thus monoclinic stacking order-in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14-18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.
RESUMEN
Two-dimensional (2D) organic-inorganic perovskite semiconductors with natural multiquantum well structures and confined 2D excitons are intriguing for the study of strong exciton-photon coupling, due to their large exciton binding energy and oscillation strength. This strong coupling leads to a formation of the half-light half-matter bosonic quasiparticle called exciton-polariton, consisting of a linear superposition state between photonic and excitonic states. Here, we demonstrate room temperature strong coupling in exfoliated wavelength-tunable 2D organic-inorganic perovskite semiconductors embedded into a planar microcavity, exhibiting large energetic splitting-to-line width ratios (>34.2). Angular-dependent spectroscopy measurements reveal that hybridized polariton states act as an ultrafast and reversible energy oscillation, involving 2D perovskite exciton, cavity modes (CM), and Bragg modes of the distributed Bragg reflector. Meanwhile, sizable hybrid particles dominantly couple to the measured optical field through the CMs. Our findings advocate a considerable promise of 2D organic-inorganic perovskite to explore fundamental quantum phenomena such as Bose-Einstein condensation, superfluidity, and exciton-polariton networks.
RESUMEN
Organic-inorganic halide perovskite semiconductors are ideal gain media for fabricating laser and photonic devices due to high absorption, photoluminescence (PL) efficiency and low nonradiative recombination losses. Herein, organic-inorganic halide perovskite CH3NH3PbI3 is embedded in the Fabry-Perot (FP) microcavity, and a wavelength-tunable excitonic lasing with a threshold of 12.9 µJ cm-2 and the spectral coherence of 0.76 nm are realized. The lasing threshold decreases and the spectral coherence enhances as the temperature decreases; these results are ascribed to the suppression of exciton irradiative recombination caused by thermal fluctuation. Moreover, both lasing and light emission below threshold from the perovskite microcavity (PM) system demonstrate a redshift with the decreasing temperature. These results provide a feasible platform based on the PM system for the study of light-matter interaction for quantum optics and the development of optoelectronic devices such as polariton lasers.
RESUMEN
Room temperature electrically pumped exciton-polariton light-emitting diode (LED) based on the n-ZnO microwire/MgO/p-GaN heterojunction was fabricated. With the injection current of 1.5 mA, the ultraviolet electroluminescence centered at wavelength of 400 nm is obtained. The whispering gallery cavity model combined with the coupling oscillator model is used to describe the emission intensity modulation, from which the strong coupling regime of the system is proved to be surviving at room temperature.
RESUMEN
Polariton lasing is the coherent emission arising from a macroscopic polariton condensate first proposed in 1996. Over the past two decades, polariton lasing has been demonstrated in a few inorganic and organic semiconductors in both low and room temperatures. Polariton lasing in inorganic materials significantly relies on sophisticated epitaxial growth of crystalline gain medium layers sandwiched by two distributed Bragg reflectors in which combating the built-in strain and mismatched thermal properties is nontrivial. On the other hand, organic active media usually suffer from large threshold density and weak nonlinearity due to the Frenkel exciton nature. Further development of polariton lasing toward technologically significant applications demand more accessible materials, ease of device fabrication, and broadly tunable emission at room temperature. Herein, we report the experimental realization of room-temperature polariton lasing based on an epitaxy-free all-inorganic cesium lead chloride perovskite nanoplatelet microcavity. Polariton lasing is unambiguously evidenced by a superlinear power dependence, macroscopic ground-state occupation, blueshift of the ground-state emission, narrowing of the line width and the buildup of long-range spatial coherence. Our work suggests considerable promise of lead halide perovskites toward large-area, low-cost, high-performance room-temperature polariton devices and coherent light sources extending from the ultraviolet to near-infrared range.
RESUMEN
Angle-resolved second harmonic generation (SHG) spectra of ZnO microwires show characteristic Fano resonances in the spectral vicinity of exciton-polariton modes. We observe a resonant peak followed by a strong dip in SHG originating from the constructive and destructive interference of the nonresonant SHG and the resonant contribution of the polariton mode. It is demonstrated that the Fano line shape, and thus the Fano asymmetry parameter q, can be tuned by the phase shift of the two channels. We develop a model to calculate the phase-dependent q as a function of the radial angle in the microwire and achieve a good agreement with the experimental results. The deduced phase-to-q relation unveils the crucial information about the dynamics of the system and offers a tool for control on the line shape of the SHG spectra in the vicinity of exciton-polariton modes.
RESUMEN
To improve the interfacial charge transfer that is crucial to the performance of perovskite solar cells, the interface engineering in a device should be rationally designed. Here we have developed an interface engineering method to tune the photovoltaic performance of planar-heterojunction perovskite solar cells by incorporating MAPbBr3-xIx (MA = CH3NH3) quantum dots (QDs) between the MAPbI3 perovskite film and the hole-transporting material (HTM) layer. By adjustment of the Br:I ratio, the as-synthesized MAPbBr3-xIx QDs show tunable fluorescence and band edge positions. When the valence band (VB) edge of MAPbBr3-xIx QDs is located below that of the MAPbI3 perovskite, the hole transfer from the MAPbI3 perovskite film to the HTM layer is hindered, and hence, the power conversion efficiency decreases. In contrast, when the VB edge of MAPbBr3-xIx QDs is located between the VB edge of the MAPbI3 perovskite film and the highest occupied molecular orbital of the HTM layer, the hole transfer from the MAPbI3 perovskite film to the HTM layer is well-facilitated, resulting in significant improvements in the fill factor, short-circuit photocurrent, and power conversion efficiency.
RESUMEN
We have developed a novel but simple approach to obtain ZnO microcombs with parallelogram stems and elongated hexagonal branches. We found that the present elongated hexagonal microcavity exhibited quite different features for its optical resonant modes due to the broken hexagonal symmetry. The resonant mode evolution of such microcavity was investigated systemically by using a spatially resolved spectroscopic technique. Theoretical analyses based on the plane wave mode and FEM simulations agreed well with the experimental results. We believe that our research allows us to have a deeper understanding of the controllable growth of novel optical cavities and the shape-dependent optical resonant modes.
RESUMEN
The optical nonlinearity of WS2 and MoS2 monolayer and few-layer films was investigated using the Z-scan technique with femtosecond pulses from the visible to the near-infrared range. The nonlinear absorption of few- and multilayer WS2 and MoS2 films and their dependences on excitation wavelength were studied. WS2 films with 1-3 layers exhibited a giant two-photon absorption (TPA) coefficient as high as (1.0 ± 0.8) × 10(4) cm/GW. TPA saturation was observed for the WS2 film with 1-3 layers and for the MoS2 film with 25-27 layers. The giant nonlinearity of WS2 and MoS2 films is attributed to a two-dimensional confinement, a giant exciton effect, and the band edge resonance of TPA.
RESUMEN
Bosons with finite lifetime exhibit condensation and lasing when their influx exceeds the lasing threshold determined by the dissipative losses. In general, different one-particle states decay differently, and the bosons are usually assumed to condense in the state with the longest lifetime. Interaction between the bosons partially neglected by such an assumption can smear the lasing threshold into a threshold domain--a stable lasing many-body state exists within certain intervals of the bosonic influxes. This recently described weak lasing regime is formed by the spontaneously symmetry breaking and phase-locking self-organization of bosonic modes, which results in an essentially many-body state with a stable balance between gains and losses. Here we report, to our knowledge, the first observation of the weak lasing phase in a one-dimensional condensate of exciton-polaritons subject to a periodic potential. Real and reciprocal space photoluminescence images demonstrate that the spatial period of the condensate is twice as large as the period of the underlying periodic potential. These experiments are realized at room temperature in a ZnO microwire deposited on a silicon grating. The period doubling takes place at a critical pumping power, whereas at a lower power polariton emission images have the same periodicity as the grating.
RESUMEN
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 44â 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.
RESUMEN
A novel ZnO microwire optical resonator with a parallelogram cross-section is fabricated, which can effectively control the light field in two dimensions. Wave-guided Fabry-Pérot modes with different polarizations are directly observed and further investigated systematically. Such a ZnO optical resonator offers another building block for the development of optoelectronic devices.
RESUMEN
High quality ZnO microcylinders (MCDs), which naturally form three-dimensional (3D) optical microcavities, were synthesized by a simple vapor transportation deposition method. The exciton-polariton effects in these 3D microcavities were investigated through the angle-resolved micro-photoluminescence (µ-PL) mappings. By using the coupled oscillator model, the 3D confinement effect of polaritons, i.e., two-dimensional (2D) whispering gallery (WG) type confinement in the cross section of the ZnO MCD, overlapping with the one-dimensional (1D) Fabry-Pérot (F-P) type confinement along the c-axis, was well interpreted.