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Perovskite solar cell (PSC) is a promising photovoltaic technology that achieves over 26% power conversion efficiency (PCE). However, the high materials costs, complicated fabrication process, as well as poor long-term stability, are stumbling blocks for the commercialization of the PSCs in normal structures. The hole transport layer (HTL)-free carbon-based PSCs (C-PSCs) are expected to overcome these challenges. However, C-PSCs have suffered from relatively low PCE due to severe energy loss at the perovskite/carbon interface. Herein, the study proposes to boost the hole extraction capability of carbon electrode by incorporating functional manganese (II III) oxide (Mn3O4). It is found that the work function (WF) of the carbon electrode can be finely tuned with different amounts of Mn3O4 addition, thus the interfacial charge transfer efficiency can be maximized. Besides, the mechanical properties of carbon electrode can also be strengthened. Finally, a PCE of 19.03% is achieved. Moreover, the device retains 90% of its initial PCE after 2000 h of storage. This study offers a feasible strategy for fabricating efficient paintable HTL-free C-PSCs.
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Considering the direct influence of substrate surface nature on perovskite (PVK) film growth, buried interfacial engineering is crucial to obtain ideal perovskite solar cells (PSCs). Herein, 1-(3-aminopropyl)-imidazole (API) is introduced at polytriarylamine (PTAA)/PVK interface to modulate the bottom property of PVK. First, the introduction of API improves the growth of PVK grains and reduces the Pb2+ defects and residual PbI2 present at the bottom of the film, contributing to the acquisition of high-quality PVK film. Besides, the presence of API can optimize the energy structure between PVK and PTAA, which facilitates the interfacial charge transfer. Density functional theory (DFT) reveals that the electron donor unit (R-C â N) of the API prefers to bind with Pb2+ traps at the PVK interface, while the formation of hydrogen bonds between the R-NH2 of API and I- strengthens the above binding ability. Consequently, the optimum API-treated inverted formamidinium-cesium (FA/Cs) PSCs yields a champion power conversion efficiency (PCE) of 22.02% and exhibited favorable stability.
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The interfacial carrier non-radiative recombination caused by buried defects in electron transport layer (ETL) material and the energy barrier severely hinders further improvement in efficiency and stability of perovskite solar cells (PSCs). In this study, the effect of the SnO2 ETL doped with choline chloride (CC), acetylcholine chloride (AC), and phosphocholine chloride sodium salt (PCSS) are investigated. These dopants modify the interface between SnO2 ETL and perovskite layer, acting as a bridge through synergistic effects to form uniform ETL films, enhance the interface contact, and passivate defects. Ultimately, compared with CC (which with âOH) and AC (which with CâO), the PCSS with PâO and sodium ions groups is more beneficial for improving performance. The device based on PCSS-doped SnO2 ETL achieves an efficiency of 23.06% with a high VOC of 1.2 V, which is considerably higher than the control device (20.55%). Moreover, after aging for 500 h at a temperature of 25 °C and relative humidity (RH) of 30-40%, the unsealed device based on SnO2-PCSS ETL maintains 94% of its initial efficiency, while the control device only 80%. This study provides a meaningful reference for the design and selection of ideal pre-buried additive molecules.
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It is well established that the collective action of assemblies of dipoles determines the electronic structure of surfaces and interfaces. This raises the question, to what extent the controlled arrangement of polar units can be used to also tune the electronic properties of the inner surfaces of materials with nanoscale pores. In the present contribution, state-of-the-art density-functional theory calculations are used to show for the prototypical case of covalent organic frameworks (COFs) that this is indeed possible. Decorating pore walls with assemblies of polar entities bonded to the building blocks of the COF layers triggers a massive change of the electrostatic energy within the pores. This, inevitably, also changes the relative alignment between electronic states in the framework and in guest molecules and is expected to have significant impacts on charge separation in COF heterojunctions, on redox reactions in COFs-based electrodes, and on (photo)catalysis.
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Perovskite solar cells (PSCs) based on the SnO2 electron transport layer (ETL) have achieved remarkable photovoltaic efficiency. However, the commercial SnO2 ETLs show various shortcomings. The SnO2 precursor is prone to agglomeration, resulting in poor morphology with numerous interface defects. Additionally, the open circuit voltage (Voc ) would be constrained by the energy level mismatch between the SnO2 and the perovskite. And, few studies designed SnO2 -based ETLs to promote crystal growth of PbI2 , a crucial prerequisite for obtaining high-quality perovskite films via the two-step method. Herein, we proposed a novel bilayer SnO2 structure that combined the atomic layer deposition (ALD) and sol-gel solution to well address the aforementioned issues. Due to the unique conformal effect of ALD-SnO2 , it can effectively modulate the roughness of FTO substrate, enhance the quality of ETL, and induce the growth of PbI2 crystal phase to develop the crystallinity of perovskite layer. Furthermore, a created built-in field of the bilayer SnO2 can help to overcome the electron accumulation at the ETL/perovskite interface, leading to a higher Voc and fill factor. Consequently, the efficiency of PSCs with ionic liquid solvent increases from 22.09% to 23.86%, maintaining 85% initial efficiency in a 20% humidity N2 environment for 1300 h.
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The power conversion efficiency (PCE) of perovskite solar cells (PSCs) can be improved through the concurrent strategies of enhancing charge transfer and passivating defects. Graphite carbon nitride (g-C3N4) has been demonstrated as a promising modifier for optimizing energy level alignment and reducing defect density in PSCs. However, its preparation process can be complicated. A simple one-step calcination approach was used in this study to prepare g-C3N4-modified TiO2via the incorporation of urea into the TiO2precursor. This modification simultaneously tunes the energy level alignment and passivates interface defects. The comprehensive research confirms that the addition of moderate amounts of g-C3N4to TiO2results in an ideal alignment of energy levels with perovskite, thereby enhancing the ability to separate and transfer charges. Additionally, the g-C3N4-modified perovskite films exhibit an increase in grain size and crystallinity, which reduces intrinsic defects density and extends charge recombination time. Therefore, the g-C3N4-modified PSC achieves a champion PCE of 20.00%, higher than that of the control PSC (17.15%). Our study provides a systematic comprehension of the interfacial engineering strategy and offers new insights into the development of high-performance PSCs.
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Image-text retrieval aims to search related results of one modality by querying another modality. As a fundamental and key problem in cross-modal retrieval, image-text retrieval is still a challenging problem owing to the complementary and imbalanced relationship between different modalities (i.e., Image and Text) and different granularities (i.e., Global-level and Local-level). However, existing works have not fully considered how to effectively mine and fuse the complementarities between images and texts at different granularities. Therefore, in this paper, we propose a hierarchical adaptive alignment network, whose contributions are as follows: (1) We propose a multi-level alignment network, which simultaneously mines global-level and local-level data, thereby enhancing the semantic association between images and texts. (2) We propose an adaptive weighted loss to flexibly optimize the image-text similarity with two stages in a unified framework. (3) We conduct extensive experiments on three public benchmark datasets (Corel 5K, Pascal Sentence, and Wiki) and compare them with eleven state-of-the-art methods. The experimental results thoroughly verify the effectiveness of our proposed method.
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Efficient energy-level alignment is crucial for achieving high performance in organic electronic devices. Because the electronic structure of an organic semiconductor is significantly influenced by its molecular orientation, comprehensively understanding the molecular orientation and electronic structure of the organic layer is essential. In this study, we investigated the interface between a 1,4,5,8,9,11-hexaazatriphenylene hexacarbonitrile (HAT-CN) hole injection layer and a zinc-phthalocyanine (ZnPc) p-type organic semiconductor. To determine the energy-level alignment and molecular orientation, we conducted in situ ultraviolet and X-ray photoelectron spectroscopies, as well as angle-resolved X-ray absorption spectroscopy. We found that the HAT-CN molecules were oriented relatively face-on (40°) in the thin (5 nm) layer, whereas they were oriented relatively edge-on (62°) in the thick (100 nm) layer. By contrast, ZnPc orientation was not significantly altered by the underlying HAT-CN orientation. The highest occupied molecular orbital (HOMO) level of ZnPc was closer to the Fermi level on the 100 nm thick HAT-CN layer than on the 5 nm thick HAT-CN layer because of the higher work function. Consequently, a considerably low energy gap between the lowest unoccupied molecular orbital level of HAT-CN and the HOMO level of ZnPc was formed in the 100 nm thick HAT-CN case. This may improve the hole injection ability of the anode system, which can be utilized in various electronic devices.
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The interface of perovskite solar cells (PSCs) plays a significant role in influencing their performance, yet there is still scarce research focusing on their difficult-to-expose bottom interfaces. Herein, ethylammonium bromide (EABr) is introduced into the bottom interface and its passivation effects are studied directly. First, EABr can improve substrate wettability, which is beneficial for the perovskite-film deposition. By lifting off the perovskite film spontaneously from the substrate, it is found that EABr can significantly reduce the amount of unreacted PbI2 at the bottom interface. These PbI2 crystals have been recently identified as a major defect source and degradation site for perovskite film. Meanwhile, EABr also lifts the valence band maximum at the bottom side of perovskite from -5.38 to -5.09 eV, facilitating better hole transfer. Such a improvement is also verified by the study of charge carrier dynamics. Through introducing EABr, all photovoltaic parameters of the inverted PSCs are improved, and their power conversion efficiency (PCE) increases from 20.41% to 21.06%. The study highlights the importance of direct characterization of the bottom interface for a better passivation effect.
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Adequately harvesting all excitons in a single molecule and inhibiting exciton losses caused by intermolecular interactions are two important factors for achieving high efficiencies thermally activated delayed fluorescence (TADF). One potential approach for optimizing these is to tune alignment of various excited state energy levels by using different doping concentrations. Unfortunately, emission efficiencies of most TADF emitters decrease rapidly with concentrations which limits the window for energy level tunning. In this work, by introducing a spiro group to increase steric hindrance of a TADF emitter (BPPXZ) with a phenoxazine and a dibenzo[a,c]phenazine, emission efficiency of the resulting molecule (BPSPXZ) is much less affected by concentration increase. This enables exploitation of the concentration effects to tune energy levels of its excited states for obtaining simultaneously small singlet-triplet energy offset and large spin-orbital coupling, leading to high-efficiency reverse intersystem crossing. With these merits, organic light-emitting diodes (OLEDs) using the BPSPXZ emitter from 5 to 60 wt% doping can all deliver EQE of over 20%. More importantly, record-high EQEs of 33.4% and 15.8% are respectively achieved in the optimized and nondoped conditions. This work proposes a strategy for developing red TADF emitters by optimizing the intermolecular interaction and energy level alignments to facilitate exciton utilization over wide doping concentrations.
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The increasing energy demand for diverse applications requires new types of devices and materials. Multifunctional materials that can fulfill different roles are of high interest as they can allow fabricating devices that can both convert and store energy. Herein, organic donor-acceptor redox polymers that can function as charge storage materials in batteries and as donor materials in bulk heterojunction (BHJ) photovoltaic devices are investigated. Based on its reversible redox chemistry, phenothiazine is used as the main building block in the conjugated copolymer design and combined with diketopyrrolopyrrol and benzothiadiazole as electron-poor comonomers to shift the optical absorption into the visible region. The resulting polymers show excellent cycling stability as positive electrode materials in lithium-organic batteries at discharge potentials of 3.6-3.7 V versus Li/Li+ as well as good performances in BHJ solar cells with up to 1.9% power conversion efficiency. This study shows that the design of such multifunctional materials is possible, however, that it also faces challenges, as essential properties for good device function can lead to diametrically opposite requirements in materials design.
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As the third generation of new thin-film solar cells, perovskite solar cells (PSCs) have attracted much attention for their excellent photovoltaic performance. Today, PSCs have reported the highest photovoltaic conversion efficiency (PCE) of 25.5%, which is an encouraging value, very close to the highest PCE of the most widely used silicon-based solar cells. However, scholars have found that PSCs have problems of being easily decomposed under ultraviolet (UV) light, poor stability, energy level mismatch and severe hysteresis, which greatly limit their industrialization. As unique materials, quantum dots (QDs) have many excellent properties and have been widely used in PSCs to address the issues mentioned above. In this article, we describe the application of various QDs as additives in different layers of PSCs, as luminescent down-shifting materials, and directly as electron transport layers (ETL), light-absorbing layers and hole transport layers (HTL). The addition of QDs optimizes the energy level arrangement within the device, expands the range of light utilization, passivates defects on the surface of the perovskite film and promotes electron and hole transport, resulting in significant improvements in both PCE and stability. We summarize in detail the role of QDs in PSCs, analyze the perspective and associated issues of QDs in PSCs, and finally offer our insights into the future direction of development.
Assuntos
Pontos Quânticos , Energia Solar , Compostos de Cálcio , Fontes de Energia Elétrica , Óxidos , TitânioRESUMO
Defects and energy offsets at the bulk and heterojunction interfaces of perovskite are detrimental to the efficiency and stability of perovskite solar cells (PSCs). Herein, we designed an amphiphilic π-conjugated ionic compound (QAPyBF4 ), implementing simultaneous defects passivation and interface energy level alignments. The p-type conjugated cations passivated the surface trap states and optimized energy alignment at the perovskite/hole transport layer. The highly electronegative [BF4 ]- enriched at the SnO2 interface featured desired band alignment due to the dipole moment of this interlayer. The planar n-i-p PSC had an efficiency of 23.1 % with Voc of 1.2â V. Notably, the synergy effect elevated the intrinsic endothermic decomposition temperature of the perovskite. The modified devices showed excellent long-term thermal (85 °C) and operational stability at the maximum power point for 1000â h at 45 °C under continuous one-sun illumination with no appreciable efficiency loss.
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Both the film quality and the electronic properties of halide perovskites have significant influences on the photovoltaic performance of perovskite solar cells (PSCs) because both of them are closely related to the charge carrier transportation, separation, and recombination processes in PSCs. In this work, an additive engineering strategy using antimony acetate (Sb(Ac)3 ) is employed to enhance the photovoltaic performance of methylammonium lead iodide (MAPbI3 )-based PSCs by improving the film quality and optimizing the photoelectronic properties of halide perovskites. It is found that Ac- and Sb3+ of Sb(Ac)3 play different roles and their synergistic effect contributed to the eventual excellent photovoltaic performance of MAPbI3 -based PSCs with a power conversion efficiency of above 21%. The Ac- anions act as a crystal growth controller and are more involved in the improvement of perovskite film morphology. By comparison, Sb3+ cations are more involved in the optimization of the electronic structure of perovskites to tailor the energy levels of the perovskite film. Furthermore, with the assistance of Sb(Ac)3 , MAPbI3 -based PSCs deliver much improved moisture, air, and thermal stability. This work can provide scientific insights on the additive engineering for improving the efficiency and long-term stability of MAPbI3 -based PSCs, facilitating the further development of perovskite-based optoelectronics.
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Flexible perovskite solar cells (f-PSCs) have been attracting tremendous attention due to their potentially commercial prospects in flexible energy system and mobile energy system. Reducing the energy barriers and charge extraction losses at the interfaces between perovskite and charge transport layers is essential to improve both efficiency and stability of f-PSCs. Herein, 4-trifluoromethylphenylethylamine iodide (CF3 PEAI) is introduced to form a 2D perovskite at the interface between perovskite and hole transport layer (HTL). It is found that the 2D perovskite plays a dual-functional role in aligning energy band between perovskite and HTL and passivating the traps in the 3D perovskite, thus reducing energy loss and charge carrier recombination at the interface, facilitating the hole transfer from perovskite to the Spiro-OMeTAD. Consequently, the photovoltaic performance of f-PSCs is significantly improved, leading to a power conversion efficiency (PCE) of 21.1% and a certified PCE of 20.5%. Furthermore, the long-term stability of f-PSCs is greatly improved through the protection of 2D perovskite layer to the underlying 3D perovskite. This work provides an excellent strategy to produce efficient and stable f-PSCs, which will accelerate their potential applications.
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Perovskite solar cells (PSCs) are important candidates for next-generation thin-film photovoltaic technology due to their superior performance in energy harvesting. At present, their photoelectric conversion efficiencies (PCEs) are comparable to those of silicon-based solar cells. PSCs usually have a multi-layer structure. Therefore, they face the problem that the energy levels between adjacent layers often mismatch each other. Meanwhile, large numbers of defects are often introduced due to the solution preparation procedures. Furthermore, the perovskite is prone to degradation under ultraviolet (UV) irradiation. These problems could degrade the efficiency and stability of PSCs. In order to solve these problems, quantum dots (QDs), a kind of low-dimensional semiconductor material, have been recently introduced into PSCs as charge transport materials, interfacial modification materials, dopants and luminescent down-shifting materials. By these strategies, the energy alignment and interfacial conditions are improved, the defects are efficiently passivated, and the instability of perovskite under UV irradiation is suppressed. So the device efficiency and stability are both improved. In this paper, we overview the recent progress of QDs' utilizations in PSCs.
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Owing to their superior thermal stability, metal halide inorganic perovskite materials continue to attract interest for photovoltaics applications. The highest reported power conversion efficiency (PCE) for solar cells based on inorganic perovskites is over 20 %. As this PCE corresponds to 73 % of the theoretical limit, there remains more room for further improving the device PCEs than for improving organic-inorganic hybrid perovskite solar cells (PSCs). The main loss is in the photovoltage, which is limited by interfaces in terms of non-radiative recombination caused by traps and energy-level mismatch. Furthermore, inefficient charge extraction at interfacial contacts reduces the photocurrent and fill factor. This Minireview summarizes the recent developments in the fundamental understanding of how the interfaces and interfacial layers influence the performance of solar cells based on inorganic perovskite absorbers. An outlook for the development of highly efficient and stable inorganic PSCs from the interface point of view is also given.
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The ability to passivate defects and modulate the interface energy-level alignment (IEA) is key to boost the performance of perovskite solar cells (PSCs). Herein, we report a robust route that simultaneously allows defect passivation and reduced energy difference between perovskite and hole transport layer (HTL) via the judicious placement of polar chlorine-terminated silane molecules at the interface. Density functional theory (DFT) points to effective passivation of the halide vacancies on perovskite surface by the silane chlorine atoms. An integrated experimental and DFT study demonstrates that the dipole layer formed by the silane molecules decreases the perovskite work function, imparting an Ohmic character to the perovskite/HTL contact. The corresponding PSCs manifest a nearly 20 % increase in power conversion efficiency over pristine devices and a markedly enhanced device stability. As such, the use of polar molecules to passivate defects and tailor the IEA in PSCs presents a promising platform to advance the performance of PSCs.
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Nanostructured tin (IV) oxide (SnO2 ) is emerging as an ideal inorganic electron transport layer in n-i-p perovskite devices, due to superior electronic and low-temperature processing properties. However, significant differences in current-voltage performance and hysteresis phenomena arise as a result of the chosen fabrication technique. This indicates enormous scope to optimize the electron transport layer (ETL), however, to date the understanding of the origin of these phenomena is lacking. Reported here is a first comparison of two common SnO2 ETLs with contrasting performance and hysteresis phenomena, with an experimental strategy to combine the beneficial properties in a bilayer ETL architecture. In doing so, this is demonstrated to eliminate room-temperature hysteresis while simultaneously attaining impressive power conversion efficiency (PCE) greater than 20%. This approach highlights a new way to design custom ETLs using functional thin-film coatings of nanomaterials with optimized characteristics for stable, efficient, perovskite solar cells.
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The efficiency of charge transport mainly depends on the interfacial energy level alignment between the conjugated polymer and the inorganic substrate. It provides an accurate understanding, predicting as well as controlling the optimal power conversion efficiency of various type of hybrid photovoltaic systems. In this article, we use hybrid functional (HSE06) to study the electronic structures and properties at the interface of poly(3-hexylthiophene)(P3HT)/CdS and P3HT/PbS for solar cell applications. We found that the dangling bonds at the inorganic surface introduce in-gap states and greatly reduce the device performance. We used pseudo-hydrogen atoms as the passivation agent to remove the dangling bonds and eliminate the in-gap states to construct the energy alignment at the hybrid interface. The calculated interfacial density of states reveal a better performance in P3HT/CdS, compared to P3HT/PbS. P3HT/CdS possesses a LUMOP3HT /CBMCdS and HOMOP3HT /VBMCdS energy offset large enough for sufficient exciton separation across the interface and prevents charge recombination. In contrast, the reason for low power conversion efficiency in P3HT/PbS lies on its HOMOP3HT /VBMPbS offset which is too small to break the exciton binding energy for charge separation. Moreover, we reported the dependency of the energy level alignment and open circuit voltage on the interfacial molecular orientations. Our DFT calculation can be used to predict candidate materials for the development of efficiency optoelectronic devices. © 2018 Wiley Periodicals, Inc.