Much recent attention has been devoted towards unraveling the microscopic optoelectronic properties of hybrid organic-inorganic perovskites. Here we investigate by coherent inelastic neutron ...scattering spectroscopy and Brillouin light scattering, low frequency acoustic phonons in four different hybrid perovskite single crystals: MAPbBr_{3}, FAPbBr_{3}, MAPbI_{3}, and α-FAPbI_{3} (MA: methylammonium, FA: formamidinium). We report a complete set of elastic constants characterized by a very soft shear modulus C_{44}. Further, a tendency towards an incipient ferroelastic transition is observed in FAPbBr_{3}. We observe a systematic lower sound group velocity in the technologically important iodide-based compounds compared to the bromide-based ones. The findings suggest that low thermal conductivity and hot phonon bottleneck phenomena are expected to be enhanced by low elastic stiffness, particularly in the case of the ultrasoft α-FAPbI_{3}.
The application of liquid‐exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene‐based organic solar cells is reported. It is shown that solution ...processing of few‐layer WS2 or MoS2 suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS2 are found to exhibit higher uniformity on ITO than those of MoS2 and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short‐circuit current (JSC), and lower series resistance than devices based on poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) and MoS2. Cells based on the ternary bulk‐heterojunction PBDB‐T‐2F:Y6:PC71BM with WS2 as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open‐circuit voltage of 0.84 V, and a JSC of 26 mA cm−2. Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS2‐based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high‐efficiency organic photovoltaics.
The use of liquid exfoliated 2D WS2 and MoS2 as hole‐transporting layers (HTLs) in ultrahigh efficiency organic solar cells is reported. WS2 yields cells with higher power conversion efficiency (PCE), fill‐factor, and short‐circuit current than MoS2 and poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate). When WS2 is introduced as HTL in PBDB‐T‐2F:Y6:PC71BM organic solar cells, a maximum PCE value of 17% is achieved.
This review article presents and discusses the recent progress made in the stabilization, protection, improvement, and design of halide perovskite‐based photocatalysts, photoelectrodes, and devices ...for solar‐to‐chemical fuel conversion. With the target of water splitting, hydrogen iodide splitting, and CO2 reduction reactions, the strategies established for halide perovskites used in photocatalytic particle‐suspension systems, photoelectrode thin‐film systems, and photovoltaic‐(photo)electrocatalysis tandem systems are organized and introduced. Moreover, recent achievements in discovering new and stable halide perovskite materials, developing protective and functional shells and layers, designing proper reaction solution systems, and tandem device configurations are emphasized and discussed. Perspectives on the future design of halide perovskite materials and devices for solar‐to‐chemical fuel conversion are provided. This review may serve as a guide for researchers interested in utilizing halide perovskite materials for solar‐to‐chemical fuel conversion.
The advancements made in the development of halide perovskites in photocatalyst particle‐suspension systems, photoelectrode thin‐film systems, and photovoltaic‐(photo)electrocatalysis systems for solar‐to‐chemical fuel conversion are reviewed. The syntheses and modification strategies established for yielding stable and efficient halide perovskites as well as the design of device configurations for water splitting, hydrogen iodide splitting, and CO2 reduction are highlighted and discussed.
Abstract In various practical situations, the information about the process distribution is sometimes partially or completely unavailable. In these instances, practitioners prefer to use ...nonparametric charts as they don’t restrict the assumption of normality or specific distribution. In this current article, a nonparametric double homogeneously weighted moving average control chart based on the Wilcoxon signed-rank statistic is developed for monitoring the location parameter of the process. The run-length profiles of the newly developed chart are obtained by using Monte Carlo simulations. Comparisons are made based on various performance metrics of run-length distribution among proposed and existing nonparametric counterparts charts. The extra quadratic loss is used to evaluate the overall performance of the proposed and existing charts. The newly developed scheme showed comparatively better results than its existing counterparts. For practical implementation of the suggested scheme, the real-world dataset related to the inside diameter of the automobile piston rings is also used.
Here we show the retrograde solubility of various hybrid perovskites through the correct choice of solvent(s) and report their solubility curves. Retrograde solubility enables to develop inverse ...temperature crystallization of FAPbX3 (FA = HC(NH2)2(+), X = Br(-)/I(-)). FAPbI3 crystals exhibit a 1.4 eV bandgap--considerably narrower than their polycrystalline counterparts.
Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA = CH3NH3(+), X = Br(-) or I(-)) have shown remarkably low trap density and charge transport properties; however, growth of ...such high-quality semiconductors is a time-consuming process. Here we present a rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX3 solubility, in certain solvents, at elevated temperatures. The crystals can be both size- and shape-controlled by manipulating the different crystallization parameters. Despite the rapidity of the method, the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPbX3 reported to date. The phenomenon of inverse or retrograde solubility and its correlated inverse temperature crystallization strategy present a major step forward for advancing the field on perovskite crystallization.
Hybrid perovskites are promising semiconductors for optoelectronic applications. However, they suffer from morphological disorder that limits their optoelectronic properties and, ultimately, device ...performance. Recently, perovskite single crystals have been shown to overcome this problem and exhibit impressive improvements: low trap density, low intrinsic carrier concentration, high mobility, and long diffusion length that outperform perovskite-based thin films. These characteristics make the material ideal for realizing photodetection that is simultaneously fast and sensitive; unfortunately, these macroscopic single crystals cannot be grown on a planar substrate, curtailing their potential for optoelectronic integration. Here we produce large-area planar-integrated films made up of large perovskite single crystals. These crystalline films exhibit mobility and diffusion length comparable with those of single crystals. Using this technique, we produced a high-performance light detector showing high gain (above 10(4) electrons per photon) and high gain-bandwidth product (above 10(8) Hz) relative to other perovskite-based optical sensors.
A two‐step ligand‐exchange strategy is developed, in which the long‐carbon‐ chain ligands on all‐inorganic perovskite (CsPbX3, X = Br, Cl) quantum dots (QDs) are replaced with halide‐ion‐pair ...ligands. Green and blue light‐emitting diodes made from the halide‐ion‐pair‐capped quantum dots exhibit high external quantum efficiencies compared with the untreated QDs.
Since compelling device efficiencies of perovskite solar cells have been achieved, investigative efforts have turned to understand other key challenges in these systems, such as engineering ...interfacial energy-level alignment and charge transfer (CT). However, these types of studies on perovskite thin-film devices are impeded by the morphological and compositional heterogeneity of the films and their ill-defined surfaces. Here, we use well-defined ligand-protected perovskite nanocrystals (NCs) as model systems to elucidate the role of heterovalent doping on charge-carrier dynamics and energy level alignment at the interface of perovskite NCs with molecular acceptors. More specifically, we develop an in situ doping approach for colloidal CsPbBr3 perovskite NCs with heterovalent Bi3+ ions by hot injection to precisely tune their band structure and excited-state dynamics. This synthetic method allowed us to map the impact of doping on CT from the NCs to different molecular acceptors. Using time-resolved spectroscopy with broadband capability, we clearly demonstrate that CT at the interface of NCs can be tuned and promoted by metal ion doping. We found that doping increases the energy difference between states of the molecular acceptor and the donor moieties, subsequently facilitating the interfacial CT process. This work highlights the key variable components not only for promoting interfacial CT in perovskites, but also for establishing a higher degree of precision and control over the surface and the interface of perovskite molecular acceptors.
Methylammonium lead iodide perovskite (MAPbI
) exhibits long charge carrier lifetimes that are linked to its high efficiency in solar cells. Yet, the mechanisms governing these unusual carrier ...dynamics are not completely understood. A leading hypothesis-disproved in this work-is that a large, static bulk Rashba effect slows down carrier recombination. Here, using second harmonic generation rotational anisotropy measurements on MAPbI
crystals, we demonstrate that the bulk structure of tetragonal MAPbI
is centrosymmetric with I4/mcm space group. Our calculations show that a significant Rashba splitting in the bandstructure requires a non-centrosymmetric lead iodide framework, and that incorrect structural relaxations are responsible for the previously predicted large Rashba effect. The small Rashba splitting allows us to compute effective masses in excellent agreement with experiment. Our findings rule out the presence of a large static Rashba effect in bulk MAPbI
, and our measurements find no evidence of dynamic Rashba effects.
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