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Mixed halide perovskites undergo phase segregation, manifested as spectral red-shifting of photoluminescence spectra under illumination. In the iodine-bromide mixed perovskites, the origin of the low-energy luminescence is related to iodine-enriched domains formation. Such domains create favorable bands for the induced carrier funneling into them. Despite the phase segregation process is crucial for mixed halide perovskite-based optoelectronics, numerous gaps exist within the understanding of this phenomenon. One such gap pertains to the emergence of temporary and intermediate photoluminescence peaks during the initial stages of phase segregation. However, these peaks appear only within the first few seconds of illumination. Nevertheless, the decreasing temperature may prolong these initial stages. In this work, we carry out a detailed study of the temperature dependence of anion segregation in MAPbBr_2I and MAPbBr2.5I0.5 halide perovskites, to obtain a deeper comprehension of segregation processes, particularly during their initial stages. The temporal evolution of low-temperature photoluminescence reveals the undergoing of the intermediate stage during the segregation process and temperature-related phase transition from orthorhombic to tetragonal phase. To complement the phase segregation study, the temperature dependence of time-resolved photoluminescence spectroscopy is provided, allowing us to estimate the change in the photoluminescence lifetimes for the initial and segregated peaks with temperature., Comment: 28 pages, 7 figures

Carrier recombination is a process that significantly influences the performance of semiconductor devices such as solar cells, photodiodes, and light-emitting diodes (LEDs). Therefore, a model that can accurately describe and quantify the net carrier recombination rate in semiconductor devices is important in order to further improve the performance of relevant semiconductor devices. The conventional model for describing the net carrier recombination rate is derived based on the condition that there is no electric current in the considered semiconductor, which is true only when the semiconductor is not part of a semiconductor device, and hence is not connected to an external circuit. The conventional model is adopted and used for describing the net carrier recombination rate in semiconductors that are part of devices (i.e. in semiconductor devices). In this paper, we derive and propose a new model for describing the net carrier recombination rate in semiconductor devices. The newly proposed model is an improvement to the currently used model by considering the fact that electric current can flow in the semiconducting materials of semiconductor devices. We validate the proposed recombination model and show that the use of the proposed model can be crucial for modeling and analyzing the performance of optoelectronic devices such as solar cells and LEDs., Comment: 26 pages, 4 figures

Organic-inorganic perovskite light-emitting devices have recently emerged as a reliable light source. Here, we developed a Single Layer Perovskite Light-Emitting Electrochemical Cells (SL-PeLEC) with laminated free-standing Carbon Nanotube Sheet (CNT) sheets as an effective charge electron injecting cathode electrode. The structure consists of bottom ITO-on-glass as a transparent electrode, the composite of CsPbBr3:PEO:LiPF6 with additive ionic salt as an emitting layer (EML) and 5 layers of CNT aerogel sheets as a top laminated cathode . Utilizing CNT free standing sheets laminated right on top of perovskite thin film in this simple single layer configuration has multiple benefits. Such CNT top cathode does not show any chemical degradation by reaction with halogens from perovskite, which is detrimental for metallic cathodes. Moreover, the formation of an internal p-i-n junction in perovskite EML composite layer by ionic migration under applied voltage bias and electric double layer (EDL) formation at each electrode interface is beneficially effecting CNT sheets by Li+ ionic doping and raises their Fermi level, further enhancing electron injection. Besides, inspired by successes of ionic additives in LECs and electrochemical doping of perovskite with alkali metals, we leveraged a lithium salt, LiPF6, within a CsPbBr3:PEO composite matrix to achieve optimal ionic redistribution and doping effects in this SL-PeLEC. Although initially CNT electrode has slightly high sheet resistance, the SL-PeLEC device has a low turn-on voltage of 2.6v and a maximum luminance intensity of 530 cd/m2, confirming the n-doping increased conductivity. This work provides a unique route toward flexible and bright perovskite LECs with stable and transparent CNT electrodes that can have injection efficiency tuned by poling induced ionic EDL-doping

Perovskite light emitting devices have drawn considerable attention for their favorable optoelectronic properties. High carrier mobilities make perovskites excellent candidates as host materials in electroluminescent devices. To achieve high performance in a simple single layer device, we employed a CsPbBr3 perovskite host and a novel ionic iridium complex guest along with a polyelectrolyte to demonstrate efficient light emitting electrochemical cells (PeLECs). For an optimal guest/host blend, 10600 cd/m2 luminance at 11.6 cd/A and 9.04 Lm/W are achieved at 4.1 V. These devices showed voltage-dependent electroluminescence color proceeding from orange-red to green, facilitated by the reconfigurable ionic materials blend. Optimized devices exhibited stable operation under constant current driving, maintaining >630 cd/m2 emission for 40 h. Our rationally-designed ionic guest at an optimal concentration of the host produced efficient (>90%) Forster energy transfer and improved thin film morphological for high performance PeLEC operation enabled by ionic migration to interfaces

A special class of anisotropic media, hyperbolic metamaterials and metasurfaces (HMMs), has attracted much attention in recent years due to its unique abilities to manipulate and engineer electromagnetic waves on the subwavelength scale. Because all HMM designs require metal dielectric composites, the unavoidable metal loss at optical frequencies inspired the development of active HMMs, where gain materials is incorporated to compensate the metal loss. Here, we experimentally demonstrate an active type II HMM that operates at vacuum wavelength near 750 nm on a silicon platform. Different from previous active HMMs operating below 1 {\mu}m, the dielectric constituent in our HMM is solely composed of gain medium, by utilizing solution processed and widely tunable metal halide perovskite gain. Thanks to the facile fabrication, tunability and silicon compatibility of our active HMM, this work paves the way towards HMM's integration into on chip components, and eventually, into photonic integrated circuits., Comment: 5 pages, 4 figures

Hybrid perovskites are emerging as highly efficient materials for optoelectronic applications, however, the operational lifetime has remained a limiting factor for the continued progress of perovskite light emitting devices such as light emitting diodes (LEDs) and perovskite light emitting electrochemical cells (PeLECs). In this work, PeLECs utilizing an optimized fraction of LiPF6 salt additive exhibit enhanced stability. At 0.5 wt% LiPF6, devices exhibit 100 h operation at high brightness in excess of 800 cd/m2 under constant current driving, achieving a maximum luminance of 3260 cd/m2 and power efficiency of 9.1 Lm/W. This performance extrapolates to a 6700 h luminance half-life from 100 cd/m2, a 5.6-fold improvement over devices with no lithium salt additive. Analysis under constant voltage driving reveals three current regimes, with lithium addition strongly enhancing current in the second and third regimes. The third regime correlates degradation of luminance with decreased current. These losses are mitigated by LiPF6 addition, an effect postulated to arise from preservation of perovskite structure. To further understand lithium salt addition, electrochemical impedance spectroscopy with equivalent circuit modeling is performed. Electrical double layer widths from ionic redistribution are minimized at 0.5wt% LiPF6 and inversely correlate with efficient performance.

Perovskite light-emitting diodes (PeLEDs) have recently attracted great research luminescence at room temperature in interest for their narrow emissions and solution processability. Remarkable progress has been achieved PeLEDs in recent years. Here we present the new configuration of ambipolar transparent perovskite light emitting device. The combination of voltage induced p-i-n formation and ionically doped carbon electrodes and allows electroluminescence in forward and reverse bias. Here we present easy-to-do transparent ambipolar light emitting subpixel based on inorganic perovskite and single wall carbon nanotubes. For this experiment PeLEDs were assembled using a glass substrate with ITO stripes as bottom electrode; spin-coated CsPbBr3/I3:PEO composite as emissive layer; single wall carbon nanotubes deposited by a simple press transfer process at room temperature. We demonstrate a concept of stacked multicolor tandem pixel. Stack of transparent light emitting units might allow fine color tuning in parallel tandem connection without segregation compared to mixed halide perovskites. This configuration conforms pixel downsizing and make to fabrication of emissive multijunction pixels in a stack.

Ionic migration in organo-halide perovskites plays an important role in operation of perovskite based solar cells and light emitting diodes. Despite the ionic migration being a reversible process, it often leads to worsening of perovskite based device performance, hysteresis in current-voltage characteristics, and phase segregation in mixed halide perovskites being as the most harmful effect. The reason is in dynamical band structure changes, which controllable engineering would solve one of the biggest challenges for development of light-emitting solar cells. Here we demonstrate controllable band bending due to migration of both cation and anion ions in mixed halide perovskite devices. The band structure rearrangement is demonstrated in light emitting solar cells based on the perovskite with organic cations methylammonium (MA+) and formamidinium (FA+), possessing non-zero dipole momentum of 2.29 and 0.21 Debye, respectively, and with PEDOT:PSS and C60 transport layers having a high barrier of 0.8 eV for charge injection. Under applied external voltage MA+ and FA+ cations move towards the electron transport layer and form a dipole layer at the perovskite/electron transport interface, which lowers threshold voltage for electroluminescence down to 1.7 V for MAPbBr2I and 2.6 V for FAPbBr2I, whereas monohalide perovskite MAPbBr3 does not demonstrate such behavior. This ability to in-situ change the device band structure paves the way developing of dual-functional devices based on simple design. It also makes mixed halide perovskites more flexible than mono halides ones for developing different optoelectronic devices without the use of special types of work function modifying transport materials.

Metal halide perovskites have emerged as promising gain materials for on-chip lasers in photonic integrated circuits (PICs). However, stable continuous wave (CW) lasing behavior under optical pumping at room temperature - a prerequisite for electrically pumped lasing - has not yet been demonstrated. To achieve stable CW operation, we introduce a multiplex of strategies that include morphological, structural and interfacial engineering of CH3NH3PbBr3 (MAPbBr3) thin films to improve perovskite's intrinsic stability, as well as high quality cavity design to reduce the operational power. We demonstrate for the first time, over 90-minute-long green CW lasing with 9.4W/cm2 threshold from a polycarbonate (PC)-defect-passivated, directly patterned MAPbBr3 two-dimensional photonic crystal (PhC) cavity without any substrate cooling. We also show our approach's effectiveness on the performance of MAPbBr3 under electrical excitation: we observe a seven-fold current efficiency enhancement by applying our strategies to a MAPbBr3 LED. This work paves the way to the realization of electrically pumped lasing in perovskites., Comment: 14 pages, 4 figures

Perovskite light-emitting diodes (PeLEDs) have drawn considerable attention for their favorable optoelectronic properties. Perovskite light-emitting electrochemical cells (PeLECs) _ devices that utilize mobile ions _ have recently been reported but have yet to reach the performance of the best PeLEDs. We leveraged a poly(ethylene oxide) electrolyte and lithium dopant in CsPbBr3 thin films to produce PeLECs of improved brightness and efficiency. In particular, we found that a single layer PeLEC from CsPbBr3:PEO:LiPF6 with 0.5% wt. LiPF6 produced highly efficient (22 cd/A) and bright (~15000 cd/m2) electroluminescence. To understand this improved performance among PeLECs, we characterized these perovskite thin films with photoluminescence (PL) spectroscopy, scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). These studies revealed that this optimal LiPF6 concentration improves electrical double layer formation, reduces the occurrence of voids, charge traps, and pinholes, and increases grain size and packing density.

All-dielectric subwavelength structures utilizing Mie resonances provide a novel paradigm in nanophotonics for controlling and manipulating light. So far, only spontaneous emission enhancement was demonstrated with single dielectric nanoantennas, whereas stimulated emission was achieved only in large lattices supporting collective modes. Here, we demonstrate the first single-particle all-dielectric monolithic nanolaser driven by Mie resonances in visible and near-IR frequency range. We employ halide perovskite CsPbBr$_3$ as both gain and resonator material that provides high optical gain (up to $\sim 10^4$ cm$^{-1}$) and allows simple chemical synthesis of nanocubes with nearly epitaxial quality. Our smallest non-plasmonic Mie-resonant single-mode nanolaser with the size of 420 nm operates at room temperatures and wavelength 535 nm with linewidth $\sim 3.5$ meV. These novel lasing nanoantennas can pave the way to multifunctional photonic designs for active control of light at the nanoscale.

Flexible, free-standing transparent conducting electrodes (TCEs) with simultaneously tunable transmittances up to 98% and sheet resistances down to 11 {\Omega}/sq were prepared by a facile spray-coating method of silver nanowires (AgNWs) onto dry-spun multiwall carbon nanotube (MWNT) aerogels. Counterintuitively, the transmittance of the hybrid electrodes can be increased as the mass density of AgNWs within the MWNT aerogels increase, however, the final achievable transmittance depends on the initial transparency of the MWNT aerogels. At the same time, a strong decrease in sheet resistance is obtained when AgNWs form a percolated network along the MWNT aerogel. Additionally, anisotropic reduction in sheet resistance and polarized transmittance of AgNWs/MWNTs aerogel is achieved with this method. The final AgNWs/MWNTs hybrid TCEs transmittance and sheet resistance can be fine-tuned by spray-coating mechanisms or by the choice of initial MWNT aerogel density. Thus, a wide range of AgNWs/MWNTs hybrid TCEs with optimized optoelectronic properties can be achieved depending of the requirements needed. Finally, the free-standing AgNWs/MWNTs hybrid TCEs can be laminated onto a wide range of substrates without the need of a bonding aid., Comment: 28 pages, 5 figures, supplemental information

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 < 2 V by exposing to Sun at open circuit Voc or at small bias voltage of Vpol ~ 1 - 2 V. Such photo-poling creates in-situ p-i-n junction via methylammonium (CH3NH3+, MA+) and I-/Br- ions migration to interfaces, lowering charge injection barriers, and self-balancing injection currents in perovskite LED. We show that before the photo-poling, the electroluminescence (EL) is highly unstable in LED regime, whereas after the photo-poling, stabilized EL exhibits unusual dynamics, increasing with time and poling cycle number, while Vth and injection current decrease with cycling runs. Additionally, photo-induced and current-induced halide segregation accumulates with cycling, that is found beneficial for LED, increasing its efficiency and brightness, but reversibly degrading photovoltaic (PV) performance, which can be easily recovered., Comment: 15 pages; 4 fisures; 1 table

Halide perovskites have emerged recently as promising materials for many applications in photovoltaics and optoelectronics. Recent studies of their optical properties suggest many novel opportunities for a design of advanced nanophotonic devices due to low-cost fabrication, high values of the refractive index, existence of excitons at room temperatures, broadband bandgap tunability, high optical gain and nonlinear response, as well as simplicity of their integration with other types of structures. This paper provides an overview of the recent progress in the study of optical effects originating from nanostructured perovskites, including their potential applications., Comment: review

We demonstrate an improvement in the performance of organic photovoltaic (OPV) systems based on small molecules by ionic gating via controlled reversible n-doping of multi-wall carbon nanotube (MWCNT) coated on fullerenes ETL: C60 and C70. Such electric double layer charging (EDLC) doping, achieved by ionic liquid (IL) charging, allows tuning the electronic concentration in MWCNT and in the fullerene planar acceptor layers, increasing it by orders of magnitude. This leads to decreasing the series and increasing the shunt resistances of OPV and allows to use of thick (up to 200 nm) ETLs, increasing the durability and stability of OPV. Two stages of OPV enhancement are described, upon the increase of gating bias Vg: at small (or even zero) Vg the extended interface of IL and porous transparent MWCNT is charged by gating, and the fullerene charge collector is significantly improved, becoming an ohmic contact. This changes the S-shaped I-V curve via improving the electron collection by n-doped MWCNT cathode with ohmic interfacial contact. The I-V curves further improve at higher gating bias Vg due to the raising of the Fermi level and lowering of MWCNT work function. At the next qualitative stage, the acceptor fullerene layer becomes n-doped by electron injection from MWCNT while ions of IL penetrate into fullerene. At this step the internal built-in field is created within OPV, which helps exciton dissociation and charge separation/transport, increasing further the Jsc and the FF (Fill factor). Overall power conversion efficiency (PCE) increases nearly 50 times in CuPc/fullerene OPV with MWCNT cathode. The concept of ionically gated MWCNT-ETL interface is numerically simulated by the drift-diffusion model which allows to fit the observed I-V curves., Comment: 34 pages, 14 figures

Solution-processed organic-inorganic lead halide perovskites have recently emerged as promising gain media for tunable semiconductor lasers, and have come to rival inorganic III-V group semiconductors as the material candidate for chip-scale lasers. Although electrically pumped lasing at room temperature is the ultimate goal, optically pumped continuous-wave lasing at room temperature,a prerequisite for a laser diode,has not been achieved so far. Here, we report lasing action in a surface emitting distributed feedback methylammonium lead iodide (MAPbI3) perovskite laser on silicon substrate, at room temperature under continuous-wave optical pumping, in ambient air environment. This outstanding performance is achieved by the ultra-low lasing threshold of 13 W/cm2, which is enabled by the thermal nanoimprint lithography that directly patterns perovskite into a high Q cavity with large mode confinement, while at the same time improves perovskite emission characteristics. Our results represent a major step toward the realization of perovskite laser diodes, which is essential in the future insertion of perovskite lasers into photonic integrated circuits, for applications in optical computing, sensing and on-chip quantum information., Comment: 16 pages, 4 figures

Using inhomogeneous Bogoliubov-de Gennes formalism we study superconducting properties of bundles of single wall carbon nanotubes, consisting of a mixture of metallic and semiconducting nanotubes, having different critical transition temperatures. We investigate how the averaged superconducting order parameter and the critical transition temperature depend on the fraction of semiconducting carbon nanotubes in the bundle.