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Although the efficiencies of all-perovskite tandem solar cells have surpassed 26%, further advancement of device performance is constrained by the large photovoltage deficit in wide-band-gap perovskite subcells. Meanwhile, state-of-the-art charge recombination layers incorporate an additional thin metal film (Au or Ag), which not only complexes device fabrication but induces parasitic optical losses. Here, we first fabricate efficient wide-band-gap perovskite solar cells (PSCs) with by suppressing nonradiative losses both in bulk material and at interface. The prepared PSCs with a band gap of 1.71 eV yield an impressive open-circuit voltage (VOC) of 1.27 V, giving a small VOC deficit of 0.44 V and an efficiency of 20.8%. We then fabricate monolithic all-printed perovskite tandem devices by constructing a metal-free recombination layer, which yields an efficiency of 23.65% and a high VOC of 2.05 V. This work offers a simple yet effective charge recombination architecture for advancing the performance of all-perovskite tandem devices.

NiOx-based inverted perovskite solar cells (PSCs) have presented great potential toward low-cost, highly efficient and stable next-generation photovoltaics. However, the presence of energy-level mismatch and contact-interface defects between hole-selective contacts (HSCs) and perovskite-active layer (PAL) still limits device efficiency improvement. Here, we report a graded configuration based on both interface-cascaded structures and p-type molecule-doped composites with two-/three-dimensional formamidinium-based triple-halide perovskites. We find that the interface defects-induced non-radiative recombination presented at HSCs/PAL interfaces is remarkably suppressed because of efficient hole extraction and transport. Moreover, a strong chemical interaction, halogen bonding and coordination bonding are found in the molecule-doped perovskite composites, which significantly suppress the formation of halide vacancy and parasitic metallic lead. As a result, NiOx-based inverted PSCs present a power-conversion-efficiency over 23% with a high fill factor of 0.84 and open-circuit voltage of 1.162 V, which are comparable to the best reported around 1.56-electron volt bandgap perovskites. Furthermore, devices with encapsulation present high operational stability over 1,200 h during T90 lifetime measurement (the time as a function of PCE decreases to 90% of its initial value) under 1-sun illumination in ambient-air conditions.

The strong anisotropic electrical properties of one-dimensional (1D) nanostructure semiconductors, especially the anisotropic carrier transport, have a negative and significant influence on the performance of solar cells if the nanostructures have random orientation. Considering the advantages of nanorod solar cells in carrier transport, we have achieved growth of vertically aligned Sb2Se3 nanorod array with highly (hk1) orientation on CdS substrate, and constructed superstrate nanorod solar cells for the first time. The Sb2Se3 nanorod array solar cells exhibit the more efficient and long-range carrier transport in vertical direction. Furthermore, in order to suppress interface recombination, a CuInSe2 quantum dots (QDs) sensitizer has been applied to fill the volume between the nanorods completely, thus forming an interpenetrating nanocomposite structure. The CuInSe2 QDs can harvest additional light by absorption of visible light and contribute photocurrent. Meantime, the QDs function as a hole transport material and thus reduce the dependence of lateral transport. Consequently, the interpenetrating nanocomposite CuInSe2/Sb2Se3 solar cells display a power conversion efficiency of 7.54% with significant enhancements in the short-circuit current density and open-circuit voltage over pure Sb2Se3 nanorod cells. This is the highest efficiency for superstrate solar cells based on Sb2Se3 nanorod arrays.

DES (Li+[(urea)3(TFSI−)1]) has a synergetic effect for regulating the interaction of ion–solvent, SEI formation and the Li+ plating reaction.

High-density electronic defects at the surfaces and grain boundaries (GBs) of perovskite materials are the major contributor to suppressing the power conversion efficiency (PCE) and deteriorating the long-term stability of the solar devices. Hence, the judicious selection of chemicals for the passivation of trap states has been regarded as an effective strategy to enhance and stabilize the photovoltaic performance of solar devices. Here, we systematically investigated the passivation effects of four organic π-conjugated phenylboronic acid molecules: phenylboronic acid, 2-amino phenylboronic acid (2a), 3-amino phenylboronic acid (3a), and 4-amino phenylboronic acid (4a) by adding them into the methylammonium lead iodide (MAPbI3) precursor solution. We found that solar devices with an optimized 5% (mol %) 3a treatment achieve the best passivation effect due to the strong cross-linking ability via hydrogen bonding interactions between the I of the [PbI6]4- octahedral network of perovskite films and the cross-linking terminal groups [-B(OH)2, (-NH2)] of 3a. Moreover, the lone pair of electrons on the N atom of an amino group of 3a can passivate the uncoordinated Pb2+ defects at the surface/GBs. As a result, the 3a-passivated device shows a high open-circuit voltage of 1.13 V, which is a 14.1% improvement compared to the control device (0.99 V). Moreover, the reduced defect density and improved carrier lifetimes enabled a high PCE of 18.89% in our blade-coated champion inverted structure of MAPbI3 solar cells, with improved long-term stability.

The use of transparent conducting oxide (TCO) as a substrate in Cu2ZnSn(S,Se)4 (CZTSSe) thin-film solar cells allows for advanced applications, such as bifacial, semi-transparent, and tandem solar cells with the capability to increase power density generation. However, the efficiency of this kind of solar cell is still below 6% based on the low-cost solution process. In this work, we develop a composition gradient strategy and demonstrate a 6.82% efficient CZTSSe solar cell on F:SnO2 (FTO) substrate under the ambient condition. The composition gradient is realized by simply depositing the precursor inks with different Zn/Sn ratios. To verify that the high performance of the solar cell is attributed to the composition gradient strategy rather than the sole change of the Zn/Sn ratio, devices based on absorbers with varied Zn/Sn ratios are fabricated. Furthermore, the structure and surface morphology of the CZTSSe films with/without composition gradients are examined. The presence of elemental gradient through the depth of the CZTSSe films before and after annealing is confirmed by secondary ion mass spectroscopy analysis. It is found that the composition gradient enhances the crystallinity of the absorber, reduces the surface roughness as well as device parasitic losses, contributing to a higher fill factor, open-circuit voltage and conversion efficiency.

In the past decades, the inverted structure (p‐i‐n structure) perovskite solar cells (PVSCs) have been attracted more by the researchers owing to their ease of fabrication, cost‐effectiveness, lower processing temperature for the fabrication of large scale and flexible devices with negligible J−V hysteresis effects. The hole transporting layer (HTL) as a major served content of PVSCs has significant influence on light harvesting, carrier extraction and transportation, perovskite crystallization, stability and cost. Generally, the organic materials are used as HTLs which have less stability due to their morphology under thermal conditions; thus, leads to change in properties of them. A tantalizing possibility is replacement of p‐type inorganic materials instead of organic materials but the plenty of options are available for inorganic HTLs. However, the development of more variants for inorganic HTL is a major challenge. Till date, many materials have been reported, but their performances have not superseded that of their organic counterparts. Herein, the review on various inorganic HTLs based inverted PVSCs has been reported and analyzed their performances with appropriate properties such as proper energy level and high carrier mobility which are not only assisted with charge transport, but also improved the stability of PVSCs under ambient conditions.

The contact quality between Si and the rear electrode and the passivation of Si play crucial roles in efficient organic/Si hybrid solar cells, especially for the open-circuit voltage (VOC). Herein,...

Defects located at the surfaces and grain boundaries of solution-processed perovskite films serve as nonradiative recombination centers and are detrimental for the photovoltaic performance of solar devices. Herein, a natural amino acid molecule methionine (Met) is selected as an effective passivation agent to enhance the optoelectronic properties of methylammonium lead iodide (MAPbI3) films. The incorporation of a small amount of Met significantly reduces the trap-state density, contributing to longer carrier lifetime of the perovskite films. As a result, solar cells made of Met-mediated perovskite films deliver a high photovoltage of 1.145 V, which is up to 100 mV higher than the control device. In addition, the Met-mediated device exhibits enhanced stability due to the reduced trap states and the improved hydrophobic property of the modified perovskite film, which retains ~ 85% of their initial efficiency after 480-h storage. The effective methionine passivation is reported, which significantly reduces the trap-state density and leads to longer carrier lifetime of the perovskite films. Methionine-mediated device produces a champion efficiency of 20.13%, with enhanced moisture stability.

Thin films of perovskite deposited from solution inevitably introduce large number of defects, which serve as recombination centers and are detrimental for solar cell performance. Although many small molecules and polymers have been delicately designed to migrate defects of perovskite films, exploiting credible passivation agents based on natural materials would offer an alternative approach. Here, an eco-friendly and cost-effective biomaterial, ploy- l -lysine (PLL), is identified to effectively passivate the defects of perovskite films prepared by blade-coating. It is found that incorporation of a small amount (2.5 mg mL−1) of PLL significantly boosts the performance of printed devices, yielding a high efficiency of 19.45% with an increase in open-circuit voltage by up to 100 mV. Density functional theory calculations combined with X-ray photoelectron spectroscopy reveal that the functional groups ( NH2, COOH) of PLL effectively migrate the Pb-I antisite defects via Pb-N coordination and suppress the formation of metallic Pb in the blade-coated perovskite film. This work suggests a viable avenue to exploit passivation agents from natural materials for preparation of high-quality perovskite layers for optoelectronic applications.

The application of doctor-blading for flexible solar cells is considerably attractive due to its potential upscaling feasibility via a roll-to-roll process. Herein, we report the fabrication of efficient flexible Cu2ZnSn(S,Se)4 (CZTSSe) solar cells by doctor-blading under ambient conditions. The device efficiency is improved from 2.22% to 5.01% by Na incorporation, while the further enhancement is limited by inhomogeneous grain growth. To address this issue, we develop an alternative blading strategy via coating Na-containing and Na-free molecular inks by turns. By carefully tailoring this combination, compact and homogeneous CZTSSe films with large grains are obtained. Meanwhile, an appropriate amount of Na incorporation is found to be beneficial for grain growth, carrier transport, and defect passivation. Consequently, a flexible device with an efficiency of 9.63% based on the doctor-blading method is achieved. This work paves the way for the future upscaling of flexible CZTSSe solar cells via low-cost solution methods.

Electronic defects at grain boundaries and surfaces of perovskite crystals impair the photovoltaic performance and stability of solar devices. In this work, we report the compensation of photovoltage losses in blade-coated methylammonium lead triiodide (MAPbI3) devices via passivation with natural amino acid (NAA) molecules. We found that the optoelectronic properties of NAA-passivated perovskite films and the corresponding device performances are closely correlated with the molecular interaction strength. A side-by-side comparative study of four typical NAAs reveals that arginine (Arg) functionalized with a guanidine end group exhibits optimum passivation effects owing to the strongest coordinative bonding with the uncoordinated Pb2+, which markedly suppresses the detrimental antisite PbI deep level defects. As a result, nonradiative charge recombination is significantly reduced, resulting in a substantially increased open-circuit voltage (VOC) of 1.17 V and a high efficiency of 20.49%. A solar module with an active area of 10.08 cm2 is also fabricated, yielding an efficiency of 15.65% with negligible VOC losses. In parallel, the Arg-passivated solar devices exhibit enhanced operational stability due to the formation of a hydrophilic Arg protective layer which encapsulates the perovskite crystals.

Formamidinium lead triiodide (FAPbI3) exhibits the smallest band gap among lead halide perovskites, which is more desirable for solar cell applications compared to methylammonium-based counterparts...

Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electrolyte during cycles. In this work, we construct a robust functional interface layer on the modified Li-B electrode which considerably improves the electrochemical stability of lithium metal electrode in solid state batteries. It is found that the functional interface layer consisting of polydioxolane, polyiodide ion and LiTFSI effectively restrains the growth of lithium dendrites through the redox shuttle reaction of I−/I3− and maintains a good contact between lithium anode and solid electrolyte during cycles. Benefit from these two advantages, the modified Li-B anode exhibits a remarkable cyclic performance in comparison with those of the bare Li-B anode.

Binary Sb

Exploration, utilization, and protection of marine resources are of great significance to the survival and development of mankind. However, currently classical optical cameras suffer information loss, low contrast, and color distortion due to the absorption and scattering nature for the underwater environment. Here, we demonstrate an underwater multispectral computational imaging system combined with single-photodetector imaging algorithm technology and a CdS/Sb

Sb2Se3 is an emerging and promising light-absorbing material with superior photovoltaic properties. However, the specific one-dimensional structure of Sb2Se3 limits the doping density, preventing a...

The optical and electrical properties of the blending organic film poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) are strongly affected by its morphology, resulting in the performance variation in Si/organic hybrid solar cells. Here, a facile postsolvent treatment is used to tailor the vertical morphology of PEDOT:PSS by introducing a nonpolar solvent. X-ray photoelectron spectroscopy depth-profiling measurements show that the distribution of PEDOT and PSS on the surface of n-type Si can be changed by nonpolar solvent n-hexane (NHX) treatment, where more PSS aggregate at the bottom of the blend film and more PEDOT float up to the top, as compared with the reference sample. As a result, after NHX treatment, the average lifetime of the Si/organic films is increased from 152 μs for untreated samples to 248 μs for NHX-treated ones because of the better passivation effect of PSS on Si. Moreover, the transmission line model measurements indicate that the contact resistance (RC) of PEDOT:PSS film and the Ag electrode is decreased for better charge collection after NHX treatment. Eventually, the best power conversion efficiency (PCE) of 13.78% for NHX-treated planar solar cells is obtained, much higher than the PCE (with best of 12.78%) of reference devices without nonpolar solvent treatment. Our results provide a facile method to tailor the vertical morphology of the PEDOT:PSS in Si/organic hybrid solar cells.

CdTe has become a leading contributor in the thin-film photovoltaic market. A suitable back contact is still one of the most crucial issues to realize efficient CdTe thin film solar cells. Herein, we intensively studied the mechanisms of interfacial modification and device performance enhancement for the representative ZnTe:Cu back contact structure. It’s found that, in spite the as-deposited ZnTe:Cu buffer could reduce the contact barrier, the device performance is still limited by the increased defect-related recombination. A controlled heat treatment process is proved to be effective in alleviating the recombination loss at the back contact. Detailed characterizations demonstrate that the CdTe/ZnTe:Cu interface reaction happens and the interfacial composition is modified during the heat treatment process, which optimize the interfacial chemical states and band alignment. The improved interfacial properties decrease the defect-related recombination and promote the holes transport, and consequently improve the device efficiency greatly.

The concept of mixed 2D/3D heterostructures has emerged as an effective method for improving the stability of lead halide perovskite solar cells, which has been, however, rarely reported in lead–ti...

In this study, nickel oxide (NiOX) thin films were prepared by direct current (DC) reactive magnetron sputtering. The various properties of NiOX thin films including deposition rate, morphology, electrical and optical properties as well as grain structure and chemical composition were systematically investigated. The material properties of NiOX were finely modified under the monitoring of target voltage during sputtering. NiOX thin films were applied as hole transport layers (HTLs) in all-inorganic CsPbI2Br perovskite solar cells (PSCs). The highest efficiency of 12.6% had been achieved for the optimized all-inorganic CsPbI2Br PSCs with the inverted structure of Glass/FTO/NiOX(HTL)/CsPbI2Br/ZnO@C60 (electron transport layer, ETL)/Ag. The PSC still yielded over 90% of its initial power output after 10 h operation without encapsulation.

Ambient air atmosphere is inimical to organic–inorganic halide perovskites and organic hole transport materials, and is, thus, necessarily avoided during device fabrication. To solve this issue, it is highly desirable to design stable perovskite-based composites and device configurations. Here, fully ambient-air and antisolvent-free-processed, stable and all-inorganic metal-oxide selective contact hole-conductor-free perovskite solar cells (HCF-PSCs) based on perovskite-based composites with an interfacial engineering strategy are reported. The formation of perovskite-based composites by interfacial engineering with carbon–graphite–CuδNi1−δO not only improved interfacial contacts, charge extraction and transport but also passivated trap states of perovskite thin films and charge recombination at the interfaces. Thus, such perovskite composites with interfacial engineering-based HCF-PSCs without encapsulation showed excellent stability by sustaining 94% of initial PCE over 300 days under ambient conditions.

Carrier loss mechanisms at microscopic regions is imperative for high-performance polycrystalline inorganic thin-film solar cells. Despite the progress on Kesterite, a promising environmental-benign and earth-abundant thin-film photovoltaic material, the microscopic carrier loss mechanisms and their impact on device performance remain unknown. Herein, we unveil these mechanisms in state-of-the-art Cu2ZnSnSe4 (CZTSe) solar cells using a framework that links microscopic-structural and optoelectronic characterizations with three-dimensional device simulations. The results indicate the CZTSe films have an encouraging intragrain minority carrier lifetime of >10 ns, a marginal radiative recombination loss through sub-band recombination and electrostatic potential fluctuation, whilst a large effective grain boundary recombination velocity of around 104 cm s-1 and a low net carrier density of ~1×1015 cm-3. We identify that severe grain boundary recombination and low net carrier density are the current limiting factors of device performance. The established framework can greatly advance the research of kesterite and other emerging photovoltaic materials.

Understanding carrier loss mechanisms at microscopic regions is imperative for the development of high-performance polycrystalline inorganic thin-film solar cells. Despite the progress achieved for kesterite, a promising environmentally benign and earth-abundant thin-film photovoltaic material, the microscopic carrier loss mechanisms and their impact on device performance remain largely unknown. Herein, we unveil these mechanisms in state-of-the-art Cu2ZnSnSe4 (CZTSe) solar cells using a framework that integrates multiple microscopic and macroscopic characterizations with three-dimensional device simulations. The results indicate the CZTSe films have a relatively long intragrain electron lifetime of 10–30 ns and small recombination losses through bandgap and/or electrostatic potential fluctuations. We identify that the effective minority carrier lifetime of CZTSe is dominated by a large grain boundary recombination velocity (~104 cm s−1), which is the major limiting factor of present device performance. These findings and the framework can greatly advance the research of kesterite and other emerging photovoltaic materials.

Flexible perovskite solar cells (f‐PSCs) have attracted increasing attention because of their enormous potential for use in consumer electronic devices. The key to achieve high device performance is to deposit pinhole‐free, uniform and defect‐less perovskite films on the rough surface of polymeric substrates. Here, a solvent engineering to tailor the crystal morphology of FA‐alloyed perovskite films prepared by one‐step blade coating is first deployed. It is found that the use of binary solvents DMF:NMP, rather than the conventional DMF:DMSO, enables to deposit dense and uniform FA‐alloyed perovskite films on both the rigid and flexible substrates. As a decisive step, an embedding 2D/3D perovskite heterostructure is in situ formed by incorporating a small amount of 4‐guanidinobutanoic acid (GBA). Accordingly, photovoltage increases up to 100 mV are realized due to the markedly suppressed nonradiative recombination, leading to high efficiencies of 21.45% and 20.16% on the rigid and flexible substrates, respectively. In parallel, improved mechanical robustness of the flexible devices is achieved due to the presence of the embedded 2D phases. The results underpin the importance of morphology control and defect passivation in delivering high‐performance flexible FA‐alloyed flexible perovskite devices., An embedding 2D/3D heterostructure is in situ formed by incorporating a small amount of 4‐guanidinobutanoic acid, which markedly suppresses nonradiative recombination, leading to high efficiencies of 21.45% and 20.16% for the rigid and flexible perovskite devices, respectively.

The persistent double layer structure whereby two layers with different properties form at the front and rear of absorbers is a critical challenge in the field of kesterite thin-film solar cells, which imposes additional nonradiative recombination in the quasi-neutral region and potential limitation to the transport of hole carriers. Herein, an effective model for growing monolayer CZTSe thin-films based on metal precursors with large grains spanning the whole film is developed. Voids and fine grain layer are avoided successfully by suppressing the formation of a Sn-rich liquid metal phase near Mo back contact during alloying, while grain coarsening is greatly promoted by enhancing mass transfer during grain growth. The desired morphology exhibits several encouraging features, including significantly reduced recombination in the quasi-neutral region that contributes to the large increase of short-circuit current, and a quasi-Ohmic back contact which is a prerequisite for high fill factor. Though this growth mode may introduce more interfacial defects which require further modification, the strategies demonstrated remove a primary obstacle toward higher efficiency kesterite solar cells, and can be applicable to morphology control with other emerging chalcogenide thin films.

High-density electronic defects at the surfaces and grain boundaries (GBs) of perovskite materials are the major contributor to suppressing the power conversion efficiency (PCE) and deteriorating the long-term stability of the solar devices. Hence, the judicious selection of chemicals for the passivation of trap states has been regarded as an effective strategy to enhance and stabilize the photovoltaic performance of solar devices. Here, we systematically investigated the passivation effects of four organic π-conjugated phenylboronic acid molecules: phenylboronic acid, 2-amino phenylboronic acid (2a), 3-amino phenylboronic acid (3a), and 4-amino phenylboronic acid (4a) by adding them into the methylammonium lead iodide (MAPbI

Indoor photovoltaics (IPVs) are expected to power the Internet of Things ecosystem, which is attracting ever-increasing attention as part of the rapidly developing distributed communications and electronics technology. The power conversion efficiency of IPVs strongly depends on the match between typical indoor light spectra and the band gap of the light absorbing layer. Therefore, band-gap tunable materials, such as metal-halide perovskites, are specifically promising candidates for approaching the indoor illumination efficiency limit of ∼56%. However, perovskite materials with ideal band gap for indoor application generally contain high bromine (Br) contents, causing inferior open-circuit voltage (V

Antimony selenide (Sb2Se3) nanorod arrays along the [001] orientation are known to transfer photogenerated carriers rapidly due to the strongly anisotropic one‐dimensional crystal structure. With advanced light‐trapping structures, the Sb2Se3 nanorod array‐based solar cells have excellent broad spectral response properties, and higher short‐circuit current density than the conventional planar structured thin film solar cells. However, the interface engineering for the Sb2Se3 nanorod array‐based solar cell is more crucial to increase the performance, because it is challenging to coat a compact buffer layer with perfect coverage to form a uniform heterojunction interface due to its large surface area and length–diameter ratio. In this work, an intermeshing In2S3 nanosheet‐CdS composite as the buffer layer, compactly coating on the Sb2Se3 nanorod surface is constructed. The application of In2S3‐CdS composite buffers build a gradient conduction band energy configuration in the Sb2Se3/buffer heterojunction interface, which reduces the interface recombination and enhances the transfer and collection of photogenerated electrons. The energy‐level regulation minimizes the open‐circuit voltage deficit at the interfaces of buffer/Sb2Se3 and buffer/ZnO layers in the Sb2Se3 solar cells. Consequently, the Sb2Se3 nanorod array solar cell based on In2S3‐CdS composite buffers achieves an efficiency of as high as 9.19% with a V OC of 461 mV., An intermeshing In2S3 nanosheet‐CdS composite buffer layer is constructed and applied in Sb2Se3 nanorod array solar cells, which build a gradient conduction band energy configuration in the Sb2Se3/buffer heterojunction interface. The champion cell based on In2S3‐CdS composite buffers achieves a PCE of 9.19% with an V OC of as high as 461 mV.

Conjugated polymers are commonly used as effective hole transport materials (HTMs) for preparation of high-performance perovskite solar cells. However, the hydrophobic nature of these materials renders it difficult to deposit photovoltaic perovskite layers on top via solution processing. In this article, we report a generic surface modification strategy that enables the deposition of uniform and dense perovskite films on top of non-wetting interfaces. In contrast to the previous proposed chemical modifications which might alter the optoelectronic properties of the interfacial layers, we realized a nondestructive surface modification enabled by introducing a layer of insulating mesoporous aluminum oxide (Al2O3). The surface energies of the typical non-wetting hole-transport layers (PTAA, P3HT, and Poly-TPD) were significantly reduced by the Al2O3 modification. Benefiting from the intact optoelectronic properties of the HTMs, perovskite solar cells deposited on these interface materials show full open-circuit voltages (VOC) with high fill factors (FF) up to 80%. Our method provides an effective avenue for exploiting the full potential of the existing as well as newly developed non-wetting interface materials for the fabrication of high-performance inverted perovskite solar cells.