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Multiphoton absorption and luminescence are fundamentally important nonlinear processes for utilizing efficient light-matter interaction. Resonant enhancement of nonlinear processes has been demonstrated for many nanostructures; however, it is believed that all higher-order processes are always much weaker than their corresponding linear processes. Here, we study multiphoton luminescence from structured surfaces and, combining multiple advantages of perovskites with the concept of metasurfaces, we demonstrate that the efficiency of nonlinear multiphoton processes can become comparable to the efficiency of the linear process. We reveal that the perovskite metasurface can enhance substantially two-photon stimulated emission with the threshold being comparable with that of the one-photon process. Our modeling of free-carrier dynamics and exciton recombination upon nonlinear photoexcitation uncovers that this effect can be attributed to the local field enhancement in structured media, a substantial increase of the mode overlap, and the selection rules of two-photon absorption in perovskites.

We study active dielectric metasurfaces composed of two-dimensional arrays of split-nanodisk resonators fabricated in InGaAsP membranes with embedded quantum wells. Depending on the geometric parameters, such split-nanodisk resonators can operate in the optical anapole regime originating from an overlap of the electric dipole and toroidal dipole Mie-resonant optical modes, thus supporting strongly localized fields and high-Q resonances. We demonstrate room-temperature lasing from the anapole lattices of engineered active metasurfaces with low threshold and high coherence.

Halide perovskite nanocrystals are a family of nanomaterials with a high prospect for use in light-emitting devices, lasers, and quantum optics, which makes their integration into photonic circuits...

The rational combination of plasmonic and all-dielectric concepts within hybrid nanomaterials provides a promising route toward devices with ultimate performance and extended modalities. Spectral matching of plasmonic and Mie-type resonances for such nanostructures can only be achieved for their dissimilar characteristic sizes, thus making the resulting hybrid nanostructure geometry complex for practical realization and large-scale replication. Here, we produced amorphous TiO2 nanospheres decorated and doped with Au nanoclusters via single-step nanosecond-laser irradiation of commercially available TiO2 nanopowders dispersed in aqueous HAuCl4. Fabricated hybrids demonstrate remarkable light-absorbing properties (averaged value ≈96%) in the visible and near-IR spectral range mediated by bandgap reduction of the laser-processed amorphous TiO2 as well as plasmon resonances of the decorating Au nanoclusters. The findings are supported by optical spectroscopy, electron energy loss spectroscopy, transmission electron microscopy, and electromagnetic modeling. Light-absorbing and plasmonic properties of the produced hybrids were implemented to demonstrate catalytically passive SERS biosensor for identification of analytes at trace concentrations and solar steam generator that permitted to increase water evaporation rate by 2.5 times compared with that of pure water under identical 1 sun irradiation conditions.

Resonant dielectric structures have emerged recently as a new platform for subwavelength nonplasmonic photonics. It was suggested and demonstrated that magnetic and electric Mie resonances can enhance substantially many effects at the nanoscale including spontaneous Raman scattering. Here, we demonstrate stimulated Raman scattering (SRS) for isolated crystalline silicon (c-Si) nanoparticles and observe experimentally a transition from spontaneous to stimulated scattering manifested in a nonlinear growth of the signal intensity above a certain pump threshold. At the Mie resonance, the light gets confined into a low volume of the resonant mode with enhanced electromagnetic fields inside the c-Si nanoparticle due to its high refractive index, which leads to an overall strong SRS signal at low pump intensities. Our finding paves the way for the development of efficient Raman nanolasers for multifunctional photonic metadevices.

The ability of light manipulation at a sub-wavelength scale of metal halide perovskite-based nanostructures through nanophotonic design were employed for advanced optical and optoelectronic applications. While these nanostructures could be efficiently tuned in the visible spectral range, their operation at infrared wavelengths is still challenging. Herein, we illustrate that islandlike films of lead-free CH3NH3SnI3 can generate strong and tunable Mie-type resonances in the near-infrared spectral range. Two critical factors contribute to the Mie resonance properties-the microscale geometry is crucial for the initiation of Mie resonances in the particles, while the concentration of free holes formed via the oxidation of Sn2+ to Sn4+ modulates the spectral position of Mie resonances. Moreover, coupling the Mie resonances to the photoluminescence peak wavelength results in the enhancement of the photoluminescence intensity. This study offers a platform for the implementation of optically resonant perovskite nanostructures as tunable light emitters for infrared photonics and optoelectronics.

Last decade, halide perovskites demonstrate high potential for efficient, tunable, and cheap photonic sources. Recently, single-particle perovskite lasers of various compositions and shapes with all dimensions close or smaller than the emitted wavelengths were demonstrated experimentally in a broad range of temperatures. In this review, we aim to cover not only the recent progress in the single-particle perovskite lasers but also provide a comprehensive analysis on strategies to achieve the most compact perovskite lasers with the best working parameters.

Nanoscale periodical chemical composition modification of different two-component compound materials GaAs, CdTe, W0.5C and TiC was realized for the first time through multi-shot femtosecond laser irradiation of their surfaces. The resulting surface modification represents periodical nanoscale ripples with different chemical composition in valleys and ridges. The underlying mechanism is related to a sequence of elementary processes, such as laser excitation surface plasmon-polariton, their interference with the incident laser radiation, inhomogeneous surface heating and incongruent cavitation-like material removal. The latter mechanism is responsible for higher evaporation rate of the components with higher volatility, resulting in growth of surface concentration of low-volatility components.

We demonstrate optically tunable control of second-harmonic generation in all dielectric nano-antennas: by using a control beam which is absorbed by the nano-resonator, we thermo-optically change the refractive index of the radiating element to modulate amplitude and phase of the second-harmonic signal. For a moderate temperature increase, sizeable modulation is demonstrated; the large tunability of the single meta-atom response paves the way to exciting avenues for reconfigurable homogeneous and heterogeneous metasurfaces.

Metasurfaces have recently enabled a further miniaturization of many optical components which are typically bulky and made of different materials. Notably, nonlinear optics in dielectric metasurfaces has been investigated achieving significant Second Harmonic (SH) generation efficiency in χ (2) materials [1] , [2] . In this work, we use a symmetry broken meta-atom shaped as an AlGaAs "nano-chair", obtained by removing one quarter of the volume from a nanocylinder with elliptic base, see Fig. 1(a) . The proposed geometry is promising for technological applications, because capable of emitting the SH light along the vertical direction ( z axis) [3] . We thus propose to use such structures in a metasurface that is concurrently excited by a Fundamental Frequency (FF) pump in the infrared region (1.55 μm) and by a Continuous Wave (CW) beam in the visible (550 nm). By varying the CW intensity, it is possible to control the temperature inside the meta-atom. The temperature increasing is responsible for a modification in the AlGaAs refractive index. Thus, by varying the CW light intensity, I 0 , we can optimize the temperature profile so as to change the refractive index of the meta-atom, achieving in such manner the tuning of the linear resonant response and consequently obtaining a detectable variation in the SH light. In Fig. 1(b) we elucidate that is possible to create a look-up table for the emitted SH magnitude and phase coming from the meta-atom as a function of I 0 . We verify that for the studied CW intensity range, the SH emission pattern preserves a main lobe ( y -polarized) towards the vertical direction with small amplitude alterations.

Bound states in the continuum (BICs) are lossless states predicted in quantum mechanics in 1929, and for the last decade, received special attention in optics and photonics as a versatile tool to achieve giant quality factors (Q factors) [1] . For ordered arrays of subwavelength meta-atoms, metasurfaces, with broken in-plane symmetry, it was shown that Q factor of quasi-BICs can be unambiguously controlled by variation of the unit cell asymmetry parameter [2] .

Organic-inorganic halide perovskites recently have emerged as a promising material for highly effective light-emitting diodes (LEDs) and solar cells (SCs). Despite efficiencies of both perovskite SCs and LEDs are already among the best, the development of a perovskite dual functional device that is capable of working in these two regimes with high efficiencies is still challenging. Here we demonstrate that the dual functional device based on mixed halide perovskite CH3NH3PbBr2I can be switched from SC to LED with low threshold voltage Vth

Tunable light-emitting nanostructures are prospective for reconfigurable compact optoelectronic devices. In this regard, halide perovskites are one of the most efficient class of materials, because of their outstanding electronic and optical properties as well as low cost of fabrication and nanostructuring. Here, we study the temperature-tunable reconfiguration of photonic modes in periodically nanostructured perovskite (MAPbI3) film probed by enhanced photoluminescence. We achieved the quality factors of resonances around 500 at wavelengths 750–760 nm. The experimental results are in well agreement with theoretical simulations. Our study reveals the origin of the emission enhancement from such kind of perovskite nanostructures and paves the way to highly directional, efficient, and tunable narowband emission from optoelectronic devices.

Halide-perovskite microlasers have demonstrated fascinating performance owing to their low-threshold lasing at room temperature and low-cost fabrication. However, being synthesized chemically, controllable fabrication of such microlasers remains challenging, and it requires template-assisted growth or complicated nanolithography. Here, we suggest and implement an approach for the fabrication of microlasers by direct laser ablation of a thin film on glass with donut-shaped femtosecond laser beams. The fabricated microlasers represent MAPbBrxIy microdisks with 760 nm thickness and diameters ranging from 2 to 9 μm that are controlled by a topological charge of the vortex beam. As a result, this method allows one to fabricate single-mode perovskite microlasers operating at room temperature in a broad spectral range (550–800 nm) with Q-factors up to 5500. High-speed fabrication and reproducibility of microdisk parameters, as well as a precise control of their location on a surface, make it possible to fabricat...

Active light-emitting all-dielectric nanoantennas recently have demonstrated great potential as highly efficient nanoscale light sources owing to their strong luminescent and Raman responses. However, their large-scale fabrication faces a number of problems related to productivity limits of existing lithography techniques. Thus, high-throughput fabrication strategies allowing in a facile way to tailor of the nanoantenna emission and thermal properties in the process of their fabrication are highly desirable for various applications. Here, we propose a cost-effective approach to large-scale fabrication of Si1−xGex alloyed Mie nanoresonators possessing an enhanced inherent Raman response which can be simply tailored via tuning the Ge concentration. Moreover, by tailoring the relative Ge composition one can gradually change a complex refractive index of the produced Si1−xGex alloy, which affects the ratio between radiative and nonradiative losses in Si1−xGex nanoantennas, which is crucial for optimization of their optical heating efficiency. Composition-tunable Si1−xGex nanoantennas with an optimized size, light-to-heat conversion and Raman response are implemented for non-invasive sensing of 4-aminothiophenol molecules with a temperature feedback modality and high subwavelength spatial resolution. The results are important for advanced multichannel optical sensing, providing information on analyte's composition, analyte-nanoantenna temperature response and spatial position.

Recent progress in submicron- and nano-fabrication technologies has led to the emergence of novel photonic structures such as optical nanoantennas and metasurfaces. Real-life applications o...

Inorganic cesium lead halide perovskite nanowires, generating laser emission in the broad spectral range at room temperature and low threshold, have become powerful tools for the cutting-edge applications in the optoelectronics and nanophotonics. However, to achieve high-quality nanowires with the outstanding optical properties, it was necessary to employ long-lasting and costly methods of their synthesis, as well as postsynthetic separation and transfer procedures that are not convenient for large-scale production. Here we report a novel approach to fabricate high-quality CsPbBr3 nanolasers obtained by rapid precipitation from dimethyl sulfoxide solution sprayed onto hydrophobic substrates at ambient conditions. The synthesis technique allows producing the well-separated nanowires with a broad size distribution of 2-50 μm in 5-7 min, being the fastest method to the best of our knowledge. The formation of nanowires occurs via ligand-assisted reprecipitation triggered by intermolecular proton transfer from (CH3)2CHOH to H2O in the presence of a minor amount of water. The XRD patterns confirm an orthorhombic crystal structure of the as-grown CsPbBr3 single nanowires. Scanning electron microscopy images reveal their regular shape and truncated pyramidal end facets, while high-resolution transmission electron microscopy ones demonstrate their single-crystal structure. The lifetime of excitonic emission of the nanowires is found to be 7 ns, when the samples are excited with energy below the lasing threshold, manifesting the low concentration of defect states. The measured nanolasers of different lengths exhibit pronounced stimulated emission above 13 μJ cm-2 excitation threshold with quality factor Q = 1017-6166. Their high performance is assumed to be related to their monocrystalline structure, low concentration of defect states, and improved end facet reflectivity.

Bound states in the continuum (BICs) represent dark modes trapped in the radiation continuum. BICs received significant attention in optics and photonics as a simple tool to achieve giant quality factors by transforming them into quasi-BICs. Here, we report the observation of high-harmonic generation in dielectric metasurfaces hosting BICs. The metasurface is composed of a square lattice with parallel Si bars of a slightly different width placed on a transparent substrate. The structure is engineered to support a quasi-BIC in the mid-IR with a high quality factor. We tune the metasurface asymmetry to enable the optimal coupling condition that provide the highest high-harmonic generation efficiency. In the experiment, we demonstrate the generation of odd optical harmonics from the 3rd to the 11th order in the BIC regime and study their polarization dependence. We measure the dependence of the high-harmonic signal on the input intensity. The concept of metasurfaces with highly localized light boosted by BIC resonances provides a new degree of freedom to control experimentally strong nonlinear optical response.

Hybrid organic&ndash, inorganic perovskites, while well examined for photovoltaic applications, remain almost completely unexplored in the terahertz (THz) range. These low-cost hybrid materials are extremely attractive for THz applications because their optoelectronic properties can be chemically engineered with relative ease. Here, we experimentally demonstrate the first attempt to apply solution-processed polycrystalline films of hybrid perovskites for the development of photoconductive terahertz emitters. By using the widely studied methylammonium-based perovskites MAPbI3 and MAPbBr3, we fabricate and characterize large-aperture photoconductive antennas. The work presented here examines polycrystalline perovskite films excited both above and below the bandgap, as well as the scaling of THz emission with the applied bias field and the optical excitation fluence. The combination of ultrafast time-resolved spectroscopy and terahertz emission experiments allows us to determine the still-debated room temperature carrier lifetime and mobility of charge carriers in halide perovskites using an alternative noninvasive method. Our results demonstrate the applicability of hybrid perovskites for the development of scalable THz photoconductive devices, making these materials competitive with conventional semiconductors for THz emission.

We design and demonstrate dramatic suppression of reflection from MAPbBr3 halide-perovskite metasurfaces. We employ the Kerker effect and engineer both electric and magnetic Mie resonances in each dielectric meta-atom to achieve a broadband performance.

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.

International audience; The full control of the fundamental photophysics of nanosystems at frequencies as high as few THz is key for tunable and ultrafast nanophotonic devices and metamaterials. Here we combine geometrical and ultrafast control of the optical properties of halide perovskite nanoparticles, which constitute a prominent platform for nanophotonics. The pulsed photoinjection of free carriers across the semiconducting gap leads to a subpicosecond modification of the far-field electromagnetic properties that is fully controlled by the geometry of the system. When the nanoparticle size is tuned so as to achieve the overlap between the narrowband excitons and the geometry-controlled Mie resonances, the ultrafast modulation of the transmittivity is completely reversed with respect to what is usually observed in nanoparticles with different sizes, in bulk systems, and in thin films. The interplay between chemical, geometrical, and ultrafast tuning offers an additional control parameter with impact on nanoantennas and ultrafast optical switches.

Inexpensive perovskite light-emitting devices fabricated by a simple wet chemical approach have recently demonstrated very prospective characteristics such as narrowband emission, low turn-on bias, high brightness, and high external quantum efficiency of electroluminescence, and have presented a good alternative to well-established technology of epitaxially grown III-V semiconducting alloys. Engineering of highly efficient perovskite light-emitting devices emitting green, red, and near-infrared light has been demonstrated in numerous reports and has faced no major fundamental limitations. On the contrary, the devices emitting blue light, in particular, based on 3D mixed-halide perovskites, suffer from electric field-induced phase separation (segregation). This crystal lattice defect-mediated phenomenon results in an undesirable color change of electroluminescence. Here we report a novel approach towards the suppression of the segregation in single-layer perovskite light-emitting electrochemical cells. Co-crystallization of direct band gap CsPb(Cl,Br)3 and indirect band gap Cs4Pb(Cl,Br)6 phases in the presence of poly(ethylene oxide) during a thin film deposition affords passivation of surface defect states and an increase in the density of photoexcited charge carriers in CsPb(Cl,Br)3 grains. Furthermore, the hexahalide phase prevents the dissociation of the emissive grains in the strong electric field during the device operation. Entirely resistant to 5.7 &times, 106 V&middot, m&minus, 1 electric field-driven segregation light-emitting electrochemical cell exhibits stable emission at wavelength 479 nm with maximum external quantum efficiency 0.7%, maximum brightness 47 cd&middot, 2, and turn-on bias of 2.5 V.

In this article, we present the pick-and-place technique for the manipulation of single nanoparticles on non-conductive substrates using a tungsten tip irradiated by a focused electron beam from a scanning electron microscope. The developed technique allowed us to perform the precise transfer of single BaTiO3 nanoparticles from one substrate to another in order to carry out measurements of elastic light scattering as well as second harmonic generation. Also, we demonstrate a fabricated structure made by finely tuning the position of a BaTiO3 nanoparticle on top of a dielectric nanowaveguide deposited on a glass substrate. The presented technique is based on the electrostatic interaction between the sharp tungsten tip charged by the electron beam and the nanoscale object. A mechanism for nanoparticle transfer to a non-conductive substrate is proposed and the forces involved in the manipulation process are evaluated. The presented technique can be widely utilized for the fabrication of nanoscale structures on optically transparent non-conductive substrates, which presents a wide range of applications for nanophotonics.

Reduction of the wavelength in on-chip light circuitry is critically important not only for the sake of keeping up with Moore's law for photonics but also for reaching toward the spectral ranges of operation of emerging materials, such as atomically thin semiconductors, vacancy-based single-photon emitters, and quantum dots. This requires efficient and tunable light sources as well as compatible waveguide networks. For the first challenge, halide perovskites are prospective materials that enable cost-efficient fabrication of micro- and nanolasers. On the other hand, III-V semiconductor nanowires are optimal for guiding of visible light as they exhibit a high refractive index as well as excellent shape and crystalline quality beneficial for strong light confinement and long-range waveguiding. Here, we develop an integrated platform for visible light that comprises gallium phosphide (GaP) nanowires directly embedded into compact CsPbBr

Plasmonic nanosponges are a powerful platform for various nanophotonic applications owing to extremely high local field enhancement in metallic nanopores. The filling of the nanopores with high-refractive index semiconductors (e.g. Si, Ge, GaP, etc.) opens up opportunities for the enhancement of nonlinear effects in these materials. However, this task remains challenging due to the lack of knowledge on the integration process of metal and high-index semiconductor components in such nanoobjects. Here, we investigate metal-dielectric nanoparticles fabricated from bilayer Si/Au films by the laser printing technique via a combination of theoretical and experimental methods. We reveal that these hybrid nanoparticles represent the Au sponge-like nanostructure filled with Si nanocrystallites. We also demonstrate that the Au net provides strong near-field enhancement in the Si grains increasing the white light photoluminescence in the hybrid nanostructures compared to uniform Si nanoparticles. These results pave the way for engineering the internal structure of the sponge-like hybrid nanoparticles possessing white light luminescence and control of their optical properties on demand.

Most of the planar light-emitting devices have a multilayer structure that consists of electron-transporting (ETL), hole- transporting (HTL), and emissive (EL) layers. Usually, the manufacturing of the devices with a complex architecture is related to the employment of expensive materials and high-tech processes such as vacuum deposition. Therefore, cost-effective and large- scale wet chemical production of efficient single-layer light-emitting devices remains a hot topic in the field of optoelectronics. Although finding a suitable semiconducting material for the engineering of such devices is challenging, inorganic cesium lead halide perovskites have recently emerged as promising candidates for this purpose. In contrast to many conventional AIII BV and AII BVI semiconductors, these perovskites exhibit room-temperature excitonic emission with high quantum yield and spectral linewidth of 14-30 nm. All of these features are required for the design of the devices demonstrating efficient light output and high color purity. So far single-layer perovskite light-emitting devices have been shown in the form of a light-emitting electrochemical cell (pero-LEC) giving bright green electroluminescence. In the meanwhile, this study has to be extended to blue and red pero-LECs to construct RGB pixels in the next-generation displays. Herein, we present the engineering of a blue pero-LEC based on inorganic perovskite-polymer composite which operates within the electrochemical doping model. We analyze the device performance to derive its crucial physical parameters and suggest a way towards its efficient and long-term operation.

Organic-halide perovskites recently have emerged as a perspective material for being used in solar cells due to their unique physical properties. One of these is ionic migration, that usually is identified as an obstacle in solar cell performance because it decreases the internal stability, which leads to device degradation. However, due to the location of defect levels of migrated ions and their vacancies under the external conditions (sun or voltage), it is possible to create of p-i-n structure inside the perovskite layer. It increases the splitting quasi-fermi level and, thus, the open-circuit voltage and efficiency. Basically, the process is reversible, and without external conditions, ions migrate backward, but if ions are fixed near the boundaries by ion-conducting polymer, it will slow down or even stop ion backward migration. In this work, we are presenting the increasing of open-circuit voltage by inserting polyethylene oxide into perovskite film.

Through the utilization of optical bound states in the continuum supported by resonant Si metasurfaces in the mid-IR spectral range, we demonstrate the generation of odd optical harmonics, from the 3rd to the 11th order.

We theoretically study the enhancement of perovskite quantum dots nonlinear photoluminescence by resonant silicon nanoparticles. Using both numerical and analytical approaches, a multifold emission efficiency enhancement in CsPbBr3 perovskite nanocrystals is predicted. Namely, we reveal the enhancement of total Purcell Factor at emission wavelength by 10 times and averaged near-field enhancement at pump wavelength by 1.5 times. Our findings can be useful for up-conversion infrared light viewers and for bioimaging.

Journal of synchrotron radiation 27(3), 625 - 632 (2020). doi:10.1107/S1600577520002192, The unique diagnostic possibilities of X-ray diffraction, small X-ray scattering and phase-contrast imaging techniques applied with high-intensity coherent X-ray synchrotron and X-ray free-electron laser radiation can only be fully realized if a sufficient dynamic range and/or spatial resolution of the detector is available. In this work, it is demonstrated that the use of lithium fluoride (LiF) as a photoluminescence (PL) imaging detector allows measuring of an X-ray diffraction image with a dynamic range of ∼107 within the sub-micrometre spatial resolution. At the PETRA III facility, the diffraction pattern created behind a circular aperture with a diameter of 5 µm irradiated by a beam with a photon energy of 500 eV was recorded on a LiF crystal. In the diffraction pattern, the accumulated dose was varied from 1.7 × 10$^5$ J cm$^{−3}$ in the central maximum to 2 × 10$^{−2}$ J cm$^{−3}$ in the 16th maximum of diffraction fringes. The period of the last fringe was measured with 0.8 µm width. The PL response of the LiF crystal being used as a detector on the irradiation dose of 500 eV photons was evaluated. For the particular model of laser-scanning confocal microscope Carl Zeiss LSM700, used for the readout of the PL signal, the calibration dependencies on the intensity of photopumping (excitation) radiation (λ = 488 nm) and the gain have been obtained., Published by Wiley-Blackwell, [S.l.]

Engineering of nonlinear optical response in nanostructures is one of the key topics in nanophotonics, as it allows for broad frequency conversion at the nanoscale. Nevertheless, the application of the developed designs is limited by either high cost of their manufacturing or low conversion efficiencies. This paper reports on the efficient second-harmonic generation in a free-standing GaP nanowire array encapsulated in a polymer membrane. Light coupling with optical resonances and field confinement in the nanowires together with high nonlinearity of GaP material yield a strong second-harmonic signal and efficient near-infrared (800-1200 nm) to visible upconversion. The fabricated nanowire-based membranes demonstrate high flexibility and semitransparency for the incident infrared radiation, allowing utilizing them for infrared imaging, which can be easily integrated into different optical schemes without disturbing the visualized beam., ACS Nano, 14 (8), ISSN:1936-0851, ISSN:1936-086X

Halide based perovskite solar cells (PSCs) have recently shown rapidly rising power conversion efficiencies up to 25.2 % [1], but there are a number of opportunities to improve their photovoltaic parameters. For example, the open current voltage (VOC) maximum of thin film cells cannot be achieved without additional photonic nanostructures, while the optimization of main SC parameters strongly depended from the transport properties of each cell layer and could be received by inclusion of nanostructures. Therefore, we employ Phosphorus doped Silicon nanoparticles (n-Si NPs) for light trapping enhancement and improved charge transfer between meso-TiO2 and MAPbI3 layers of PSCs. We show the efficiency growth from 17.6 to 18.2% via the improvement of VOC. The proposed method for preparing upgraded PSCs is cheap and can be simply implemented to the technological process.

Over the last five years, inorganic lead halide perovskite nanowires have emerged as prospective candidates to supersede standard semiconductor analogs in advanced photonic designs and optoelectronic devices. In particular, CsPbX3 (X = Cl, Br, I) perovskite materials have great advantages over conventional semiconductors such as defect tolerance, highly efficient luminescence, and the ability to form regularly shaped nano- and microcavities from solution via fast crystallization. However, on the way of electrically pumped lasing, the perovskite nanowires grown on transparent conductive substrates usually suffer from strong undesirable light leakage increasing their threshold of lasing. Here, we report on the integration of CsPbBr3 nanowires with nanostructured indium tin oxide substrates possessing near-unity effective refractive index and high conductivity by using a simple wet chemical approach. Surface passivation of the substrates is found out to govern the regularity of the perovskite resonators’ shape. The nanowires show room-temperature lasing with ultrahigh quality factors (up to 7860) which are up to four times higher than that of similar structures on a flat indium tin oxide layer, resulting in more than twofold reduction of the lasing threshold for the nanostructured substrate. Numerical modeling of eigenmodes of the nanowires confirms the key role of low-refractive-index substrate for improved light confinement in the Fabry–Pérot cavity which results in superior laser performance.

Local optical heating and Raman nanothermometry based on resonant silicon particles provide a new promising platform for a number of key nanophotonics applications associated with thermally induced processes at the nano- and microscale. In this work, the crystallization of amorphous silicon nanodisks with optical resonances caused by local optical heating has been studied. The crystallization process is controlled by Raman microspectroscopy. The crystallization temperature of a single nanodisk of about 900 K has been determined under the action of a strongly focused cw laser beam. As a result, an annealed resonant silicon nanoparticle has allowed controlled and reversible heating in the temperature range of 300–1000 K with the possibility of mapping the heating region with submicron spatial resolution.

High-throughput laser printing of resonant silicon nanoparticles has emerged as a novel tool for the fabrication of deeply subwavelength objects with various functionalities. The applications of resonant silicon nanoparticles crucially depend on their crystalline state. However, the ways to control the crystalline structure during laser printing remain unstudied. Here we demonstrate, both experimentally and theoretically, how the crystalline structure of silicon nanoparticles fabricated by a laser printing technique can be varied from almost amorphous to a polycrystalline state. In particular, we propose a method of crystalline structure control via changing the distance between the irradiated silicon film and the receiving substrate. This study allows the most optimal conditions for second harmonic generation to be revealed. We believe that the proposed method opens the door to fully controllable laser printing of functional nanoparticles and nanostructures.

Ultrafast plasmonics of novel materials has emerged as a promising field of nanophotonics bringing new concepts for advanced optical applications. Ultrafast electronic photoexcitation of a diamond surface and subsequent surface plasmon-polaritons (SPPs) excitation are studied both theoretically and experimentally - for the first time. After photoexcitation on the rising edge of the pulse, transient surface metallization was found to occur for laser intensity near 18 TW/cm$^2$ due to enhancement of the impact ionization rate; in this regime, the dielectric constant of the photoexcited diamond becomes negative in the trailing edge of the pulse thereby increasing the efficacy with which surface roughness leads to inhomogeneous energy absorption at the SPP wave-vector. These transient SPP waves imprint permanent fine and coarse surface ripples oriented perpendicularly to the laser polarization. The theoretical modeling is supported by the experiments on the generation of laser-induced periodic surface structure on diamond surface with normally incident 515-nm, 200-fs laser pulses. Sub-wavelength ($\Lambda \approx 100$ nm) and near wavelength ($\Lambda \approx 450$ nm) surface ripples oriented perpendicularly to the laser polarization emerged within the ablative craters with the increased number of laser shots; the spatial periods of the surface ripples decrease with the increasing exposure following known cumulative trends. The comparison between experimental data and theoretical predictions makes evident the role of transient changes of the dielectric permittivity of diamond during the initial stage of periodic surface ripple formation upon irradiation with ultrashort laser pulses., Comment: 11 pages, 14 figures, has been resubmitted to PRB

Since Complementary metal–oxide–semiconductor technology is the conventional technology for micro- and optoelectronics, integration of emerging materials, such as halide perovskites, into the process is an important branch of perovskite technologies development. In this regard ITO free device research becomes increasingly important. The Perovskite Light-Emitting electrochemical cells are a promising alternative to conventional Perovskite Light Emitting Diodes. In this work we demonstrate green (λEL = 523 nm) CsPbBr3 Perovskite Light-Emitting electrochemical cells with luminescence intensity of 50 kd/m2 integrated with Si++(111) substrate.

These days halide perovskite is a very popular material to be applied both in photovoltaics and photonics due to its unique properties and low-cost methods of fabrication. High photoluminescence quantum yield and good nonlinear coefficients of perovskite material allow achieving multiphoton absorption in perovskite. Encapsulation of perovskite quantum dots in polymer matrix enables to prevent interaction with the environment and increase the material lifetime. In this paper, we present a semitransparent visualizer of infrared lasers working on two-photon absorption in halide perovskite nanocrystals encapsulated in the polymer matrix.

In the recent years, semiconductor and dielectric nanophotonic structures attracted a lot of attention for their resonant optical properties finding applications in thermal tuning and optical heating. Exciting high quality optical modes of both electric and magnetic nature in nanoresonators of high-index materials, one can effectively enhance optical absorption in such structures. Another big advantage of semiconductor materials is the ability to finely control the level of optical losses in visible and near infrared (near-IR) range through varying the doping level. In this work, we show theoretically that by moderate carrier doping of silicon via donors from group V materials one can achieve effective heating of nanoresonators. We show that by tuning the doping level of crystalline silicon supporting high quality non-radiative modes based on quasi bound states in the continuum one can achieve strong heating in near-IR under continuous wave regime illumination. We believe that our finding will pave the way for an efficient semiconductor near-IR all-optical sensors and nanoheaters.

We develop a model describing non-equilibrium processes under the excitation of resonant semiconductor nanostructures with ultrashort laser pulses with a duration of about 100 fs. We focus on the heating effects related to pulsed excitation with account on free carriers generation, thermalization, and relaxation. The heat exchange between the electron and phonon system is treated within the two-temperature model. We applied the developed model to describing pulsed heating of silicon nanocylinder on top of a dielectric substrate. We come up with estimations of the thermal damage threshold of the considered structures which provides the limits for the experimental conditions and ensures thermal stability of the samples.

In this work we develop the concept of integrated light source based on halide perovskite microwires for Bloch surface waves (BSWs) in one-dimensional photonic crystals. We theoretically study modes supported by a CsPbBr3 microwire placed on the surface of a photonic crystal. The modes with field distribution similar to BSW are observed. We study the coupling of microwire modes with BSWs depending on the geometric parameters of the wire. BSW excitation efficiency exceeding 40% is found for BSW-like modes of microwire. We also examine resonant modes of finite microwire and show that BSW-like modes play a main role in the excitation of BSWs with perovskite radiation. Our research paves the way for the implementation of complete integrated optical setups on the surface of photonic crystals.

Using direct femtosecond-laser projection lithography in chemically synthesized CsPbBr3 perovskite microcrystals we demonstrate high-throughput fabrication of advanced binary microscale optical elements for nanofocusing as well as generation of high-order optical vortex beams. The obtained results highlight the CsPbBr3 microcrystals as a promising material for realization of various complicated 2D micro-optical elements and holograms that can be directly imprinted using non-destructive and practically relevant laser technologies.

All-dielectric nanophotonics is a powerful tool for improvement of thin-film optoelectronic devices because of low optical losses, strong light localization, and chemical robustness against such materials as halide perovskites. However, large-scale and low-cost approaches to create functional nanostructures are still not developed. In our work, we show a novel method to create mesoporous electron transport layer based on optically resonant silicon nanoparticles incorporated into TiO 2 paste to be applied for perovskite (MAPbI 3 ) solar cell. The inclusion of Mie-resonant silicon nanoparticles helps to improve light absorption by a perovskite layer without reduction of the active material. The management of Si nanoantennas concentration provides to reach a power conversion efficiency higher than 21% by increasing all main device parameters. Our multi-physical theoretical simulations of the solar cells with the resonant silicon nanoparticles provide physical understanding on the mechanisms of the device improvement as well as help to optimize the silicon nanoparticles concentration.

Nonlinear harmonic generation in nanostructures is one of the key topics in nanophotonics, as it allows infrared-to-visible light conversion at the nanoscale.his work reports on the efficient third-harmonic generation in a free-standing Si nanowire array encapsulated into a polymer membrane. High nonlinearity of Si material X 31112.45 ≈ 10 –19m2 /V 2 and light coupling with optical resonances in the nanowires yield a strong third-harmonic signal and efficient infrared (1200 — 2000nm) to visible (400 — 666nm) upconversion. The fabricated membranes demonstrate high flexibility and semitransparency, which makes them convenient to use as visualizers.

Structured environments are employed in a plethora of applications to tailor dynamics of light–matter interaction processes by modifying the structure of electromagnetic fields. The promising example of such a system is antiresonant photonic crystal fibers (AR-PCFs), which allow light–analyte interactions in a very long channel. Here we probe contribution of microstructuring and nontrivial mode hierarchy on light–matter interactions in AR-PCFs by investigating lifetime shortening of perovskite ( CsPbBr 3 ) nanocrystals grown to fiber capillaries. The crystals have been deposited using a wet chemistry approach and then excited by a supercontinuum source in the 450–500 nm range. Emission spectra have been measured and analyzed via the time-correlated single photon counting (TCSPC) technique, unravelling contributions of core and cladding modes. Fluorescence lifetime imaging inside an AR-PCF enables mapping input of various electromagnetic channels into light–matter interaction processes. Our results pave the way for tailoring the dynamics of high-order quantum processes, promoting the concept of AR-PCF as a light-driven reactor.