Indoor Self-Powered Perovskite Optoelectronics with Ultraflexible Monochromatic Light Source.

Self-powered skin optoelectronics fabricated on ultrathin polymer films is emerging as one of the most promising components for the next-generation Internet of Things (IoT) technology. However, a longstanding challenge is the device underperformance owing to the low process temperature of polymer substrates. In addition, broadband electroluminescence (EL) based on organic or polymer semiconductors inevitably suffers from periodic spectral distortion due to Fabry-Pérot (FP) interference upon substrate bending, preventing advanced applications. Here, ultraflexible skin optoelectronics integrating high-performance solar cells and monochromatic light-emitting diodes using solution-processed perovskite semiconductors is presented. n-i-p perovskite solar cells and perovskite nanocrystal light-emitting diodes (PNC-LEDs), with power-conversion and current efficiencies of 18.2% and 15.2 cd A-1 , respectively, are demonstrated on ultrathin polymer substrates with high thermal stability, which is a record-high efficiency for ultraflexible perovskite solar cell. The narrowband EL with a full width at half-maximum of 23 nm successfully eliminates FP interference, yielding bending-insensitive spectra even under 50% of mechanical compression. Photo-plethysmography using the skin optoelectronic device demonstrates a signal selectivity of 98.2% at 87 bpm pulse. The results presented here pave the way to inexpensive and high-performance ultrathin optoelectronics for self-powered applications such as wearable displays and indoor IoT sensors.

Carrier Dynamics of Efficient Triplet Harvesting in AgBiS2 /Pentacene Singlet Fission Solar Cells.

Singlet fission is a process by which an organic semiconductor is able to generate two triplet excitons from a single photon. If charges from the triplets can be successfully harvested without heavy losses in energy, then this process can enable a single-junction solar cell to surpass the Shockley-Queisser limit. While singlet fission processes are commonly observed in several materials, harvesting the resulting triplets is difficult and has been demonstrated with only a few transport materials. Here, transient absorption spectroscopy is used to investigate singlet fission and carrier transfer processes at the AgBiS2 /pentacene (AgBiS2 /Pc) heterojunction. The successful transfer of triplets from pentacene to AgBiS2 and the transfer of holes from AgBiS2 to pentacene is observed. Further singlet fission in pentacene by modifying the crystallinity of the pentacene layer and have fabricated the first singlet fission AgBiS2 /Pc solar cell is enhanced. Singlet fission devices exhibit higher external quantum efficiency compared with the control devices, and thus demonstrating the significant contribution of charges from the singlet fission process.

Solution-Processed Red, Green, and Blue Quantum Rod Light-Emitting Diodes.

Solution-processed semiconductor nanocrystals are evolving as potential candidates for future display and lighting applications owing to their size-tunable emission, ultrasaturated colors, and compatibility with large-area flexible substrates. Among them, quantum rods (QRs) are emerging materials for optoelectronic applications, offering polarized emission, high light outcoupling efficiency, color purity, and better stability in solid films. However, synthesizing QRs covering the full visible wavelength region has been a big challenge, particularly in the blue range. Herein, we report for the first time the synthesis of red CdSe/CdS, green CdSe/ZnxCd1-xS/ZnS, and blue CdSe/ZnxCd1-xS/ZnS QRs and their application in red, green, and blue QR-based light-emitting diodes (QR-LEDs). We have improved the charge injection balance into the QRs through embedding a poly(methyl methacrylate) (PMMA) layer between the emissive and electron transport layers. The thin PMMA electron-blocking layer (EBL) suppresses the excessive electron flux and thus promotes charge injection balance and pushes the recombination zone back to the QR layer, resulting in 1.35×, 1.2×, and 1.7× peak external quantum efficiency improvement for red, green, and blue QR-LEDs, respectively. The efficiency roll-off of green and blue QR-LEDs with an EBL is less than 50% at maximum current density. The proposed red, green, and blue QR-LEDs open up an avenue toward further improving the light source efficiency and stability focusing on real device applications.

Solution-Processed, Inverted AgBiS2 Nanocrystal Solar Cells.

AgBiS2 nanocrystals are a promising nontoxic alternative to PbS, CsPbI3, and CdS quantum dots for solution-fabricated nanocrystal photovoltaics. In this work, we fabricated the first inverted (p-i-n) structure AgBiS2 nanocrystal solar cells. We selected spray-coated NiO as the hole-transporting material and used PCBM/BCP as the electron-transporting material. Combining transient photocurrent and photovoltage measurements with femtosecond transient absorption spectroscopy, we investigated the charge collection process on metal oxide/AgBiS2 interfaces and demonstrated that the NiO/AgBiS2 NC junction in the p-i-n configuration is more efficient for charge carrier collection. The fabricated p-i-n solar cells exhibited a 4.3% power conversion efficiency (PCE), which was higher than that of conventional n-i-p solar cells fabricated using the same sample. Additionally, inverted devices showed an ultrahigh short-circuit current (JSC) over 20.7 mA cm-2 and 0.38 V open-circuit voltage (VOC), suggesting their potential for further improvements in efficiency and, eventually, for large-scale production.

Optically Clear Films of Formamidinium Lead Bromide Perovskite for Wide-Band-Gap, Solution-Processed, Semitransparent Solar Cells.

Solvent engineering and antisolvent methods have been used extensively to achieve high-quality, homogeneous, and crystalline perovskite thin films. Usually, highly concentrated (>1.1 M) precursor solutions are used to achieve the maximum power conversion efficiency (PCE), and most fabrication studies focus on iodide-based metal halide perovskites (MHPs). However, high concentrations of precursors are not suitable for semitransparent (ST) MHP solar cells (STPSCs), which require thinner films to achieve a high average visible transmittance (AVT). The deposition of high-quality perovskites with variable concentrations in a one-step method is challenging due to the complexity of the antisolvent crystallization process. Here, we have developed an in situ technique based on photoluminescence (PL) measurements to identify the optimum delay time for antisolvent crystallization in formamidinium lead bromide (FAPbBr3). By monitoring the in situ PL, the nucleation, crystal growth, and early perovskite formation phases are easily identified for a range of concentrations. Subsequently, we fabricated opaque and ST solar cells with optically clear, ST perovskite films formed from precursors with varying concentrations. These all-solution-processed STPSCs achieved AVTs of up to 35.6, 42.5, and 49.2%, with the corresponding PCEs of 5.71, 3.25, and 1.86% in p-i-n type, FAPbBr3 perovskite solar cells with transparent Ag nanowire electrodes. These devices show good stability over several weeks and an impressive Voc as high as 1.24 V for STPSCs and 1.38 V for opaque cells produced with a thick Ag electrode. This work demonstrates the potential use of in situ spectroscopy to tailor the film growth of halide perovskites with varying concentrations and the feasibility of using wide-band-gap perovskites for ST solar cells with exceptional clarity and higher Voc.

Photorechargeable Lead-Free Perovskite Lithium-Ion Batteries Using Hexagonal Cs3Bi2I9 Nanosheets.

Materials that enable bifunctional operation in harvesting and storing energy are currently in high demand, due to their potential to efficiently use renewable solar energy. Here, we present a lead-free, all-inorganic, bismuth-based perovskite halide, which acts as a photoelectrode that can harvest energy under illumination without the assistance of an external load in a lithium-ion battery. The battery performance is shown using three different current collectors: copper, fluorine-doped tin oxide (FTO) and carbon felt (CF) to exhibit the electrode's function as a normal coin cell, as a basic photobattery with a transparent collector to elucidate its functional mechanism, and as an optimized photobattery displaying competitive metrics with other photobatteries obtaining a photo conversion efficiency of ∼0.43% for the first discharge. Upon discharging under illumination, we observed an increase in capacity from 410 to 975 mA·h·g-1. Further exploration in anode structure and design provides a path toward more efficient photobatteries.

Quantum-Dot Tandem Solar Cells Based on a Solution-Processed Nanoparticle Intermediate Layer.

Tandem cells are one of the most effective ways of breaking the single junction Shockley-Queisser limit. Solution-processable phosphate-buffered saline (PbS) quantum dots are good candidates for producing multiple junction solar cells because of their size-tunable band gap. The intermediate recombination layer (RL) connecting the subcells in a tandem solar cell is crucial for device performance because it determines the charge recombination efficiency and electrical resistance. In this work, a solution-processed ultrathin NiO and Ag nanoparticle film serves as an intermediate layer to enhance the charge recombination efficiency in PbS QD dual-junction tandem solar cells. The champion devices with device architecture of indium tin oxide/S-ZnO/1.45 eV PbS-PbI2/PbS-EDT/NiO/Ag NP/ZnO NP/1.22 eV PbS-PbI2/PbS-EDT/Au deliver a 7.1% power conversion efficiency, which outperforms the optimized reference subcells. This result underscores the critical role of an appropriate nanocrystalline RL in producing high-performance solution-processed PbS QD tandem cells.