Halide perovskite nanowire-based lasers have become a powerful tool for modern nanophotonics, being deeply subwavelength in cross-section and demonstrating low-threshold lasing within the whole ...visible spectral range owing to the huge gain of material even at room temperature. However, their emission directivity remains poorly controlled because of the efficient outcoupling of radiation through their subwavelength facets working as pointlike light sources. Here, we achieve directional lasing from a single perovskite CsPbBr3 nanowire by imprinting a nanograting on its surface, which provides stimulated emission outcoupling to its vertical direction with a divergence angle around 2°. The nanopatterning is carried out by the high-throughput laser ablation method, which preserves the luminescent properties of the material that is typically deteriorated after processing via conventional lithographic approaches. Moreover, nanopatterning of the perovskite nanowire is found to decrease the number of the lasing modes with a 2-fold increase of the quality factor of the remaining modes.
Ultrafast all-optical modulation with optically resonant nanostructures is an essential technology for high-speed signal processing on a compact optical chip. Key challenges that exist in this field ...are relatively low and slow modulations in the visible range as well as the use of expensive materials. Here we develop an ultrafast all-optical modulator based on MAPbBr3 perovskite metasurface supporting exciton–polariton states with exceptional points. The additional angular and spectral filtering of the modulated light transmitted through the designed metasurface allows us to achieve 2500% optical signal modulation with the shortest modulation time of 440 fs at the pump fluence of ∼40 μJ/cm2. Such a value of the modulation depth is record-high among the existing modulators in the visible range, while the main physical effect behind it is polariton condensation. Scalable and cheap metasurface fabrication via nanoimprint lithography along with the simplicity of perovskite synthesis and deposition make the developed approach promising for real-life applications.
Detection of hazardous volatile organic and inorganic species is a crucial task for addressing human safety in the chemical industry. Among these species, there are hydrogen halides (HX, X = Cl, Br, ...I) vastly exploited in numerous technological processes. Therefore, the development of a cost-effective, highly sensitive detector selective to any HX gas is of particular interest. Herein, we demonstrate the optical detection of hydrogen chloride gas with solution-processed halide perovskite nanowire lasers grown on a nanostructured alumina substrate. An anion exchange reaction between a CsPbBr3 nanowire and vaporized HCl molecules results in the formation of a structure consisting of a bromide core and thin mixed-halide CsPb(Cl,Br)3 shell. The shell has a lower refractive index than the core does. Therefore, the formation and further expansion of the shell reduce the field confinement for experimentally observed laser modes and provokes an increase in their frequency. This phenomenon is confirmed by the coherency of the data derived from XPS spectroscopy, EDX analysis, in situ XRD experiments, HRTEM images, and fluorescent microspectroscopy, as well as numerical modeling for Cl– ion diffusion and the shell-thickness-dependent spectral position of eigenmodes in a core–shell perovskite nanowire. The revealed optical response allows the detection of HCl molecules in the 5–500 ppm range. The observed spectral tunability of the perovskite nanowire lasers can be employed not only for sensing but also for their precise spectral tuning.
Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton–exciton interactions. ...In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of the exciton–exciton interaction, making materials with the highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow overcoming this limitation. Namely, we demonstrate a record-high value of the nonlinear optical response in the nanostructured organic–inorganic halide perovskite MAPbI3, experimentally detected as a 19.7 meV blueshift of the polariton branch under femtosecond laser irradiation. This is substantially higher than characteristic values for the samples based on conventional semiconductors and monolayers of transition-metal dichalcogenides. The observed strong polaron-enhanced nonlinearity exists for both tetragonal and orthorhombic phases of MAPbI3 and remains stable at elevated temperatures.
Halide perovskite nanomaterials are widely used in optoelectronics and photonics due to their outstanding luminescent properties, whereas their strong multiphoton absorption makes them prospective ...for bioimaging. Nonetheless, instability of perovskites in aqueous solutions is an important limitation that prevents their application in biology and medicine. Here, we demonstrate fluorescence and upconversion imaging in living cells by employing CsPbBr3 nanocrystals (NCs) that show an improved water-resistance (at least for 24 h) after their coating as individual particles with various silica-based shells. The obtained phTEOS-TMOS@CsPbBr3 NCs possess high quality, which we confirm with high-resolution transmission and scanning transmission electron microscopy, X-ray diffraction analysis, Fourier-transform infrared and energy-dispersive X-ray spectroscopies, as well as with fluorescence optical microscopy. The developed platform can make the halide perovskite NCs suitable for various bioimaging applications.
Luminescent composites based on entirely non-toxic, environmentally friendly compounds are in high demand for a variety of applications in photonics and optoelectronics. Carbon dots are a recently ...developed kind of luminescent nanomaterial that is eco-friendly, biocompatible, easy-to-obtain, and inexpensive, with a stable and widely tunable emission. Herein, we introduce luminescent composites based on carbon dots of different chemical compositions and with different functional groups at the surface which were embedded in a nanoporous silicate glass. The structure and optical properties of these composites were comprehensively examined using electron microscopy, Fourier transform infrared transmission, UV-Vis absorption, and steady-state and time-resolved photoluminescence. It is shown that the silicate matrix efficiently preserved, and even enhanced the emission of different kinds of carbon dots tested. The photoluminescence quantum yield of the fabricated nanocomposite materials reached 35–40%, which is comparable to or even exceeds the values for carbon dots in solution.
The integration of nanoparticles (NPs) into functional materials is a powerful tool for the smart engineering of their physical properties. If properly designed and optimized, NPs possess unique ...optical, electrical, quantum, and other effects that will improve the efficiency of optoelectronic devices. Here, we propose a novel approach for the enhancement of perovskite light-emitting diodes (PeLEDs) based on electronic band structure deformation by core-shell NPs forming a metal-oxide-semiconductor (MOS) structure with an Au core and SiO2 shell located in the perovskite layer. The presence of the MOS interface enables favorable charge distribution in the active layer through the formation of hole transporting channels. For the PeLED design, we consider integration of the core-shell NPs in the realistic numerical model. Using our verified model, we show that, compared with the bare structure, the incorporation of NPs increases the radiative recombination rate of PeLED by several orders of magnitude. It is intended that this study will open new perspectives for further efficiency enhancement of perovskite-based optoelectronic devices with NPs.
Mixed-halide perovskite allows to realize conception of light-emitting solar cell (LESC) due to possibility to in-situ change device band structure by formation of dipole layer under applied voltage ...and intrinsic properties of perovskite ions. LESC has optimized perovskite-based solar cell (SC) architecture, but light-emitting diode (LED) regime performances is still low. Defect passivation can improve LED efficiencies due to reducing nonradiative recombination via defect levels. Solvent annealing allows to regulate film formation process and leads to better morphology and grain size for our application. Defect density is significantly reduced due to this passivation method. Here we demonstrate effect of annealing in vapors of dimethylformamide (DMF), dimethyl sulfoxide (DMSO) and acetonitrile (MeCN) atmosphere on LESC photovoltaic characteristic, electroluminescence (EL) peak wavelength and photoluminescence quantum yield (PLQY) of mixed-halide perovskite film.
Abstract
Tetramethyl orthosilicate and triethoxyphenylsilane, which contains hydrophobic phenyl groups, were used as a silica (SiO2) source in a modified ligand-assisted reprecipitation synthesis ...approach for the fabrication of water-stable perovskite nanocrystals. Hydrolysis-condensation reaction of tetramethyl orthosilicate and triethoxyphenylsilane results in a formation of 3D siloxane network. Employing triethoxyphenylsilane in the synthesis enhances the hydrophobic properties of the SiO2 shell, which increases the stability of perovskites in aqueous medium. The stability of the CsPbBr3@SiO2 nanocrystals was estimated after 24 h of water exposure by the photoluminescence measurements at different time points. The synthesized CsPbBr3@SiO2 nanocrystals were visualized during
in vitro
experiments with murine melanoma B16-F10 cells. Hence, the potential of CsPbBr@SiO2 nanocrystals for bioimaging purposes was observed.
Deeply subwavelength lasers (or nanolasers) are highly demanded for compact on-chip bioimaging and sensing at the nanoscale. One of the main obstacles for the development of single-particle ...nanolasers with all three dimensions shorter than the emitting wavelength in the visible range is the high lasing thresholds and the resulting overheating. Here we exploit exciton-polariton condensation and mirror-image Mie modes in a cuboid CsPbBr3 nanoparticle to achieve coherent emission at the visible wavelength of around 0.53 μm from its ultra-small (≈0.007 μm3 or ≈λ3/20) semiconductor nanocavity. The polaritonic nature of the emission from the nanocavity localized in all three dimensions is proven by direct comparison with corresponding one-dimensional and two-dimensional waveguiding systems with similar material parameters. Such a deeply subwavelength nanolaser is enabled not only by the high values for exciton binding energy (≈35 meV), refractive index (>2.5 at low temperature), and luminescence quantum yield of CsPbBr3, but also by the optimization of polaritons condensation on the Mie resonances with quality factors improved by the metallic substrate. Moreover, the key parameters for optimal lasing conditions are intermode free spectral range and phonons spectrum in CsPbBr3, which govern polaritons condensation path. Such chemically synthesized colloidal CsPbBr3 nanolasers can be potentially deposited on arbitrary surfaces, which makes them a versatile tool for integration with various on-chip systems.