Despite a recent shift toward methylammonium (MA)-free lead-halide perovskites for perovskite solar cells, high-efficiency formamidinium lead iodide (FAPbI) devices still often require methylammonium chloride (MACl) as an additive, which evaporates away during the annealing process. In this article, it is shown that the residual MA, however, triggers thermal instability. To investigate the possibility of an optimal concentration of MA that may improve thermal stability, the intrinsic thermal stability of pure FA, FA-rich, MA-rich, and pure MA perovskite films (FAMAPbI, FAMA) is studied.
View Article and Find Full Text PDFQuantum cutting (QC) allows the conversion of high-energy photons into lower-energy photons, exhibiting great potential for infrared communications. Yb-doped perovskite nanocrystals can achieve an efficient QC process with extremely high photoluminescence quantum yield (PLQY) thanks to the favorable Yb incorporation in the perovskite structure. However, conventionally used oleic acid-oleylamine-based ligand pairs cause instability issues due to highly dynamic binding to surface states that have curbed their potential applications.
View Article and Find Full Text PDFThe ability to perceive color by the retina can be attributed to both its trichromatic photoreceptors and the antagonistic neural wiring known as the opponent process. While neuromorphic sensors have been shown to demonstrate memory and adaptation capabilities, color perception is still challenging due to the intrinsic lack of spectral selectivity in narrow bandgap semiconductors. Furthermore, research on emulating neural wiring is severely lacking.
View Article and Find Full Text PDFColloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr QDs. However, this also increases the fluorescence intermittency.
View Article and Find Full Text PDFThe power conversion efficiency (PCE) of the state-of-the-art large-area slot-die-coated perovskite solar cells (PSCs) is now over 19%, but issues with their stability persist owing to significant intrinsic point defects and a mass of surface imperfections introduced during the fabrication process. Herein, the utilization of a hydrophobic all-organic salt is reported to modify the top surface of large-area slot-die-coated methylammonium (MA)-free halide perovskite layers. Bearing two molecules, each of which is endowed with anchoring groups capable of exhibiting secondary interactions with the perovskite surfaces, the organic salt acts as a molecular lock by effectively binding to both anion and cation vacancies, substantially enhancing the materials' intrinsic stability against different stimuli.
View Article and Find Full Text PDFRuddlesden-Popper (RP) perovskites have been gaining traction in the development of high-efficiency or blue-emitting perovskite light emitting diodes (PeLEDs) due to the unique energy funneling mechanism, which enhances photoluminescence intensity, and dimensional control, which enables spectral tuning. In a conventional p-i-n device structure, the quality of RP perovskite films, including grain morphology and defects, as well as device performance can be significantly influenced by the underlying hole-transport layer (HTL). Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is commonly used in several PeLEDs as an HTL because of its high electrical conductivity and optical transparency.
View Article and Find Full Text PDFDefect management strategies are vital for enhancing the performance of perovskite-based optoelectronic devices, such as perovskite-based light-emitting diodes (PeLEDs). As additives can fucntion both as acrystallization modifier and/or defect passivator, a thorough study on the roles of additives is essential, especially for blue emissive Pe-LEDs, where the emission is strictly controlled by the -domain distribution of the Ruddlesden-Popper (RP, LAPbX, where L refers to a bulky cation, while A and X are monovalent cation, and halide anion, respectively) perovskite films. Of the various additives that are available, octyl phosphonic acid (OPA) is of immense interest because of its ability to bind with uncoordinated Pb ( notorious for nonradiative recombination) and therefore passivates them.
View Article and Find Full Text PDFExtending halide perovskites' optoelectronic properties to stimuli-responsive chromism enables switchable optoelectronics, information display, and smart window applications. Here, we demonstrate a band gap tunability (chromism) via crystal structure transformation from three-dimensional FAPbBr to a ⟨110⟩ oriented FAPbBr structure using a mono-halide/cation composition (FA/Pb) tuning. Furthermore, we illustrate reversible photochromism in halide perovskite by modulating the intermediate phase in the FAPbBr structure, enabling greater control of the optical band gap and luminescence of a ⟨110⟩ oriented mono-halide/cation perovskite.
View Article and Find Full Text PDFThe rapid emergence of organic-inorganic lead halide perovskites for low-cost and high-efficiency photovoltaics promises to impact new photovoltaic concepts. Their high power conversion efficiencies, ability to coat perovskite layers on glass via various scalable deposition techniques, excellent optoelectronic properties, and synthetic versatility for modulating transparency and color allow perovskite solar cells (PSCs) to be an ideal solution for building-integrated photovoltaics (BIPVs), which transforms windows or façades into electric power generators. In this review, the unique features and properties of PSCs for BIPV application are accessed.
View Article and Find Full Text PDFHeterostructures, combining perovskite nanocrystals (PNC) and chalcogenide quantum dots, could pave a path to optoelectronic device applications by enabling absorption in the near-infrared region, tailorable electronic properties, and stable crystal structures. Ideally, the heterostructure host material requires a similar lattice constant as the guest which is also constrained by the synthesis protocol and materials selectivity. Herein, we present an efficient one-pot hot-injection method to synthesize colloidal all-inorganic cesium lead halide-lead sulfide (CsPbX (X = Cl, Br, I)-PbS) heterostructure nanocrystals (HNCs) via the epitaxial growth of the perovskite onto the presynthesized PbS nanocrystals (NCs).
View Article and Find Full Text PDFIn less than a decade, organic-inorganic metal halide perovskites (MHPs) have shown tremendous progress in the field of light-emitting applications. Perovskite light-emitting diodes (PeLEDs) have reached external quantum efficiencies (EQE) exceeding 20 % and they have been recognized as a potential contender of the commercial display technologies. However, perovskite thin films in PeLEDs are generally deposited via a spin-coating process, which is not favourable for large area device fabrication.
View Article and Find Full Text PDFJ Phys Chem Lett
February 2021
In the past few years, a large variety of perovskite solar cells (PSCs) with vivid and well-distinguished color hues have been demonstrated. In this Perspective, we compare different strategies employed to realize colorful PSCs both in opaque and semitransparent designs. The approaches used to modulate the PSCs' colorful appearance can be divided into two main categories: the first one based on the modifications of their internal layers (, absorber, electron- and/or hole-transporting layers, and electrodes), while the second is based on the addition of external colored or nanostructured films to the standard PSCs.
View Article and Find Full Text PDFSurface imperfections created during fabrication of halide perovskite (HP) films could induce formation of various defect sites that affect device performance and stability. In this work, all-organic surface modifiers consisting of alkylammonium cations and alkanoate anions are introduced on top of the HP layer to passivate interfacial vacancies and improve moisture tolerance. Passivation using alkylammonium alkanoate does not induce formation of low-dimensional perovskites species.
View Article and Find Full Text PDFMetal lead halide perovskite nanocrystals have emerged as promising candidates for optoelectronic applications. However, the inclusion of toxic lead is a major concern for the commercial viability of these materials. Herein, we introduce a new family of non-toxic reduced dimension RbCuX (X = Br, Cl) colloidal nanocrystals with one-dimensional crystal structure consisting [CuX] ribbons isolated by Rb cations.
View Article and Find Full Text PDFRealization of reduced ionic (cationic and anionic) defects at the surface and grain boundaries (GBs) of perovskite films is vital to boost the power conversion efficiency of organic-inorganic halide perovskite (OIHP) solar cells. Although numerous strategies have been developed, effective passivation still remains a great challenge due to the complexity and diversity of these defects. Herein, a solid-state interdiffusion process using multi-cation hybrid halide perovskite quantum dots (QDs) is introduced as a strategy to heal the ionic defects at the surface and GBs.
View Article and Find Full Text PDFAn amendment to this paper has been published and can be accessed via a link at the top of the paper.
View Article and Find Full Text PDFTo overcome the drawbacks in three-dimensional (3D) perovskites, such as instability, surface hydration, and ion migration, recently researchers have focused on comparatively stable lower-dimensional perovskite derivatives. All-inorganic zero-dimensional (0D) perovskites (, CsPbX; X = Cl, Br, I) can be evolved as a high performing material due to their larger exciton binding energy and better structural stability. The clear understanding of carrier recombination process in 0D perovskites is very important for better exploitation in light-emitting devices.
View Article and Find Full Text PDFSlow hot carrier cooling in halide perovskites holds the key to the development of hot carrier (HC) perovskite solar cells. For accurate modeling and pragmatic design of HC materials and devices, it is essential that HC temperatures are reliably determined. A common approach involves fitting the high-energy tail of the main photobleaching peak in a transient absorption spectrum with a Maxwell-Boltzmann distribution.
View Article and Find Full Text PDFMetal halide perovskite solar cells, despite achieving high power conversion efficiency (PCE), need to demonstrate high stability prior to be considered for industrialization. Prolonged exposure to heat, light, and moisture is known to deteriorate the perovskite material owing to the breakdown of the crystal structure into its non-photoactive components. In this study, we show that by combining the organic ligand 1-naphthylmethylammoinium iodide (NMAI) with methylammonium (MA) to form a mixed dimensional (NMA)(MA)PbI perovskite the optical, crystallographic and morphological properties of the newly formed mixed dimensional perovskite films under thermal ageing can be retained.
View Article and Find Full Text PDFThe recent emergence of lead halide perovskites as ionic-electronic coupled semiconductors motivates the investigation of alternative solution-processable materials with similar modulatable ionic and electronic transport properties. Here, a novel semiconductor-cubic NaSbS -for ionic-electronic coupled transport is investigated through a combined theoretical and experimental approach. The material exhibits mixed ionic-electronic conductivity in inert atmosphere and superionic conductivity in humid air.
View Article and Find Full Text PDFRecently, semitransparent perovskite solar cells (ST-PSCs) have received overwhelming attention due to their potential applications in building-integrated photovoltaics (BIPV) and in tandem solar cells. The best ST-PSCs, despite the high efficiency achieved, still show limited bifacial properties and lack esthetic properties. Here, we have demonstrated efficient bifacial colorful ST-PSCs using copper thiocyanate (CuSCN), as a hole-transporting material, in an n-i-p architecture.
View Article and Find Full Text PDFEfficient perovskite light-emitting diodes are designed by employing an ordered vertical domain distribution in quasi-two-dimensional (quasi-2D) perovskites to induce better electron flow to the emitting domains. Dimethyl sulfoxide is added to the precursor solution to tune the crystallization rate and promote the formation of high- domains near the substrate surface via the one-step deposition method. Optimized deposition conditions yielding a film with favorable energetic landscape for both carrier injection and confinement results in a 4-fold external quantum efficiency (EQE) enhancement with maximum EQE of 5.
View Article and Find Full Text PDFHalide perovskites are promising materials for development in hot carrier (HC) solar cells, where the excess energy of above-bandgap photons is harvested before being wasted as heat to enhance device efficiency. Presently, HC separation and transfer processes at higher-energy states remain poorly understood. Here, we investigate the excited state dynamics in CHNHPbI using pump-push-probe spectroscopy.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2019
Tandem solar cells (SCs) based on perovskite and silicon represent an exciting possibility for a breakthrough in photovoltaics, enhancing SC power conversion efficiency (PCE) beyond the single-junction limit while keeping the production cost low. A critical aspect to push the tandem PCE close to its theoretical limit is the development of high-performing semitransparent perovskite top cells, which also allow suitable near-infrared transmission. Here, we have developed highly efficient semitransparent perovskite SCs (PSCs) based on both mesoporous and planar architectures, employing Cs(MAFA)Pb(IBr) and FACsPbIBr perovskites with band gaps of 1.
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