Highly Efficient and Bendable Organic Solar Cells with Solution‐Processed Silver Nanowire Electrodes

Highly efficient and bendable organic solar cells (OSCs) are fabricated using solution‐processed silver nanowire (Ag NW) electrodes. The Ag NW films were highly transparent (diffusive transmittance ≈ 95% at a wavelength of 550 nm), highly conductive (sheet resistance ≈ 10 Ω sq^?1), and highly flexible (change in resistance ≈ 1.1 ± 1% at a bending radius of ≈200 μm). Power conversion efficiencies of ≈5.80 and 5.02% were obtained for devices fabricated on Ag NWs/glass and Ag NWs/poly(ethylene terephthalate) (PET), respectively. Moreover, the bendable devices fabricated using the Ag NWs/PET films decrease slightly in their efficiency (to ≈96% of the initial value) even after the devices had been bent 1000 times with a radius of ≈1.5 mm.     

HPbI3: A New Precursor Compound for Highly Efficient Solution‐Processed Perovskite Solar Cells

Recently, there have been extensive research efforts on developing high performance organolead halide based perovskite solar cells. While most studies focused on optimizing the deposition processes of the perovskite films, the selection of the precursors has been rather limited to the lead halide/methylammonium (or formamidium) halide combination. In this work, we developed a new precursor, HPbI₃, to replace lead halide. The new precursor enables formation of highly uniform formamidium lead iodide (FAPbI₃) films through a one‐step spin‐coating process. Furthermore, the FAPbI₃ perovskite films exhibit a highly crystalline phase with strong (110) preferred orientation and excellent thermal stability. The planar heterojunction solar cells based on these perovskite films exhibit an average efficiency of 15.4% and champion efficiency of 17.5% under AM 1.5 G illumination. By comparing the morphology and formation process of the perovskite films fabricated from the formamidium iodide (FAI)/HPbI₃, FAI/PbI₂, and FAI/PbI₂ with HI additive precursor combinations, it is shown that the superior property of the HPbI₃ based perovskite films may originate from 1) a slow crystallization process involving exchange of H⁺ and FA⁺ ions in the PbI₆ octahedral framework and 2) elimination of water in the precursor solution state.     

Achieving 20% Efficiency for Low‐Temperature‐Processed Inverted Perovskite Solar Cells

Low‐temperature‐processed inverted perovskite solar cells (PVSCs) attract increasing attention because they can be fabricated on both rigid and flexible substrates. For these devices, hole‐transporting layers (HTLs) play an important role in achieving efficient and stable inverted PVSCs by adjusting the anodic work function, hole extraction, and interfacial charge recombination. Here, the use of a low‐temperature (≤150 °C) solution‐processed ultrathin film of poly[(9,9‐dioctyl‐fluorenyl‐2,7‐diyl)‐co‐(4,4′‐(N‐(4‐secbutylphenyl) diphenylamine)] (TFB) is reported as an HTL in one‐step‐processed CH₃NH₃PbI₃ (MAPbI₃)‐based inverted PVSCs. The fabricated device exhibits power conversion efficiency (PCE) as high as 20.2% when measured under AM 1.5 G illumination. This PCE makes them one of the MAPbI₃‐based inverted PVSCs that have the highest efficiency reported to date. Moreover, this inverted PVSC also shows good stability, which can retain 90% of its original efficiency after 30 days of storage in ambient air.     

Fully Solution‐Processed Small Molecule Semitransparent Solar Cells: Optimization of Transparent Cathode Architecture and Four Absorbing Layers

Semitransparent solar cells (SSCs) can open photovoltaic applications in many commercial areas, such as power‐generating windows and building integrated photovoltaics. This study successfully demonstrates solution‐processed small molecule SSCs with a conventional configuration for the presently tested material systems, namely BDTT‐S‐TR:PC₇₀BM, N(Ph‐2T‐DCN‐Et)₃:PC₇₀BM, SMPV1:PC₇₀BM, and UU07:PC₆₀BM. The top transparent cathode coated through solution processes employs a highly transparent silver nanowire as electrode together with a combination interface bilayer of zinc oxide nanoparticles (ZnO) and a perylene diimide derivative (PDINO). This ZnO/PDINO bilayer not only serves as an effective cathode buffer layer but also acts as a protective film on top of the active layer. With this integrated contribution, this study achieves a power conversion efficiency (PCE) of 3.62% for fully solution‐processed SSCs based on BDTT‐S‐TR system. Furthermore, the other three systems with various colors exhibited the PCEs close to 3% as expected from simulations, demonstrate the practicality and versatility of this printed semitransparent device architecture for small mole­cule systems. This work amplifies the potential of small molecule solar cells for window integration.     

Solution‐Processed Bulk‐Heterojunction Solar Cells Based on Monodisperse Dendritic Oligothiophenes

A novel family of soluble conjugated dendritic oligothiophenes (DOTs) as monodisperse 3D macromolecular architectures was characterized with respect to optical and redox properties in solution and in solid films. Band gaps of 2.5–2.2 eV, typical for organic semiconductors, were determined as well as HOMO/LUMO energy levels ideal for efficient electron transfer to acceptors such as [6,6]‐phenyl‐C₆₁‐butyric acid methyl ester (PCBM) identifying them as suitable materials for solar cell applications. Solution‐processed bulk‐heterojunction solar cells using DOTs as electron donor and PCBM as acceptor were prepared and investigated. High open‐circuit voltages V_OC of 1.0 V and power‐conversion efficiencies up to 1.72% were obtained for the DOT‐based devices. The higher generations DOTs provide the highest efficiencies. Based on the monodispersity of the DOTs, an analysis of the molar ratio between donor and acceptor in the blended film was possible leading to an optimal value of five to six thiophene units per PCBM.     

Probing Molecular and Crystalline Orientation in Solution‐Processed Perovskite Solar Cells

The microstructure of solution‐processed organometallic lead halide perovskite thin films prepared by the “gas‐assisted” method is investigated with synchrotron‐based techniques. Using a combination of GIWAXS and NEXAFS spectroscopy the orientational alignment of CH₃NH₃PbI₃ crystallites and CH₃NH₃⁺ cations are separately probed. The GIWAXS results reveal a lack of preferential orientation of CH₃NH₃PbI₃ crystallites in 200–250 nm thick films prepared on both planar TiO₂ and mesoporous TiO₂. Relatively high efficiencies are observed for device based on such films, with 14.3% achieved for planar devices and 12% for mesoporous devices suggesting that highly oriented crystallites are not crucial for good cell performance. Oriented crystallites however are observed in thinner films (≈60 nm) deposited on planar TiO₂ (but not on mesoporous TiO₂) indicating that the formation of oriented crystallites is sensitive to the kinetics of solvent evaporation and the underlying TiO₂ morphology. NEXAFS measurements on all samples found that CH₃NH₃⁺ cations exhibit a random molecular orientation with respect to the substrate. The lack of any NEXAFS dichroism for the thin CH₃NH₃PbI₃ layer deposited on planar TiO₂ in particular indicates the absence of any preferential orientation of CH₃NH₃⁺ cations within the CH₃NH₃PbI₃ unit cell for as‐prepared layers, that is, without any electrical poling.     

Efficient Perovskite Hybrid Solar Cells via Ionomer Interfacial Engineering

The surface of the solution‐processed methylammonium lead tri‐iodide (CH₃NH₃PbI₃) perovskite layer in perovskite hybrid solar cells (pero‐HSCs) tends to become rough during operation, which inevitably leads to deterioration of the contact between the perovskite layer and the charge‐extraction layers. Moreover, the low electrical conductivity of the electron extraction layer (EEL) gives rises to low electron collection efficiency and severe charge carrier recombination, resulting in energy loss during the charge‐extraction and ‐transport processes, lowering the efficiency of pero‐HSCs. To circumvent these problems, we utilize a solution‐processed ultrathin layer of a ionomer, 4‐lithium styrenesulfonic acid/styrene copolymer (LiSPS), to re‐engineer the interface of CH₃NH₃PbI₃ in planar heterojunction (PHJ) pero‐HSCs. As a result, PHJ pero‐HSCs are achieved with an increased photocurrent density of 20.90 mA cm^?2, an enlarged fill factor of 77.80%, a corresponding enhanced power conversion efficiency of 13.83%, high reproducibility, and low photocurrent hysteresis. Further investigation into the optical and electrical properties and the thin‐film morphologies of CH₃NH₃PbI₃ with and without LiSPS, and the photophysics of the pero‐HSCs with and without LiSPS are shown. These demonstrate that the high performance of the pero‐HSCs incorporated with LiSPS can be attributed to the reduction in both the charge carrier recombination and leakage current, as well as more efficient charge carrier collection, filling of the perforations in CH₃NH₃PbI_3, and a higher electrical conductivity of the LiSPS thin layer. These results demonstrate that our method provides a simple way to boost the efficiency of pero‐HSCs.     

Solution‐Processed Organic Tandem Solar Cells

A solution‐processed polymer tandem cell fabricated by stacking two single cells in series is demonstrated. The two bulk‐heterojunction subcells have complementary absorption maxima at λ_max ～ 850 nm and λ_max ～ 550 nm, respectively. A composite middle electrode is applied that serves both as a charge‐recombination center and as a protecting layer for the first cell during spin‐coating of the second cell. The subcells are electronically coupled in series, which leads to a high open‐circuit voltage of 1.4 V, equal to the sum of each subcell. The layer thickness of the first (bottom) cell is tuned to maximize the optical absorption of the second (top) cell. The performance of the tandem cell is presently limited by the relatively low photocurrent generation in the small‐bandgap polymer of the top cell. The combination of our tandem architecture with more efficient small‐bandgap materials will enable the realization of highly efficient organic solar cells in the near future.     

Amino Acid-Induced Interface Charge Engineering Enables Highly Reversible Zn Anode

Despite the impressive merits of low-cost and high-safety electrochemical energy storage for aqueous zinc ion batteries, researchers have long struggled against the unresolved issues of dendrite growth and the side reactions of zinc metal anodes. Herein, a new strategy of zinc-electrolyte interface charge engineering induced by amino acid additives is demonstrated for highly reversible zinc plating/stripping. Through electrostatic preferential absorption of positively charged arginine molecules on the surface of the zinc metal anode, a self-adaptive zinc-electrolyte interface is established for the inhibition of water adsorption/hydrogen evolution and the guidance of uniform zinc deposition. Consequently, an ultra-long stable cycling up to 2200 h at a high current density of 5 mA cm⁻² is achieved under an areal capacity of 4 mAh cm⁻². Even cycled at an ultra-high current density of 10 mA cm⁻², 900 h-long stable cycling is still demonstrated, demonstrating the reliable self-adaptive feature of the zinc-electrolyte interface. This work provides a new perspective of interface charge engineering in realizing highly reversible bulk zinc anode that can prompt its practical application in aqueous rechargeable zinc batteries.     

Film Morphology of High Efficiency Solution‐Processed Small‐Molecule Solar Cells

Morphological control over the bulk heterojunction (BHJ) microstructure of a high‐efficiency small molecule photovoltaic system is demonstrated using both thermal treatment and solvent additive processing. Single crystal X‐ray diffraction is utilized to understand molecular interactions in the solid state and the BHJ morphology is examined using bright field, high‐resolution, and cross‐section transmission electron microscopy techniques. Controlling the domain size, while maintaining good molecular order within the semiconducting donor material, is found to be crucial in achieving high performance and over 90% internal quantum efficiency exhibited under the optimized conditions.     

All‐Solution‐Processed Random Si Nanopyramids for Excellent Light Trapping in Ultrathin Solar Cells

Si nanopyramids have been suggested as one of the most promising Si nanostructures to realize high‐efficient ultrathin solar cells or photodetectors due to their low surface area enhancement and outstanding ability to enhance light absorption. However, the present techniques to fabricate Si nanopyramids are either complex or expensive. In parallel, disordered nanostructures are believed to be extremely effective to realize broadband light trapping for solar cells. Here, a simple and cost‐effective method is presented to form random Si nanopyramids based on an all‐solution process, the mechanism behind which is the successful transfer of the generation site of bubbles from Si surface to the introduced Ag nanoparticles so that OH^? can react with the entire Si surface to naturally form random and dense Si nucleus. For optical performance, it is experimentally demonstrated that the random Si nanopyramid textured ultrathin crystalline Si (c‐Si) can achieve light trapping approaching the Lambertian limit. Importantly, it is revealed, by numerical calculations, that random Si nanopyramids outperform periodic ones on broadband light absorption due to more excited optical resonance modes. The finding provides a new opportunity to improve the performance of ultrathin c‐Si solar cells with a simpler process and lower cost.     

Over 16.7% Efficiency Organic‐Silicon Heterojunction Solar Cells with Solution‐Processed Dopant‐Free Contacts for Both Polarities

Realization of synchronous improvement in optical management and electrical engineering is necessary to achieve high‐performance photovoltaic device. However, inherent challenges are faced in organic‐silicon heterojunction solar cells (HSCs) due to the poor contact property of polymer on structured silicon surface. Herein, a remarkable efficiency boost from 12.6% to over 16.7% in poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate)/n‐silicon (PEDOT:PSS/n‐Si) HSCs by independent optimization of hole‐/electron‐selective contacts only relying on solution‐based processes is realized. A bilayer PEDOT:PSS film with different functionalizations is utilized to synchronously realize conformal contact and effective carrier collection on textured Si surface, making the photogenerated carriers be well separated at heterojunction interface. Meanwhile, fullerene derivative is used as electron‐transporting layer at the rear n‐Si/Al interface to reduce the contact barrier. The study of carriers' transport and independent optimization on separately contacted layers may lead to an effective and simplified path to fabricate high‐performance organic‐silicon heterojunction devices.     

A Versatile Fluoro‐Containing Low‐Bandgap Polymer for Efficient Semitransparent and Tandem Polymer Solar Cells

The versatility of a fluoro‐containing low band‐gap polymer, poly[2,6‐(4,4‐bis(2‐ethylhexyl)‐4H‐cyclopenta[2,1‐b;3,4‐b’]dithiophene)‐alt‐4,7‐(5‐fluoro‐2,1,3‐benzothia‐diazole)] (PCPDTFBT) in organic photovoltaics (OPVs) applications is demonstrated. High boiling point 1,3,5‐trichlorobenzene (TCB) is used as a solvent to manipulate PCPDTFBT:[6,6]‐phenyl‐C₇₁‐butyric acid methyl ester (PC₇₁BM) active layer morphology to obtain high‐performance single‐junction devices. It promotes the crystallization of PCPDTFBT polymer, thus improving the charge‐transport properties of the active layer. By combining the morphological manipulation with interfacial optimization and device engineering, the single‐junction device exhibits both good air stability and high power‐conversion efficiency (PCE, of 6.6%). This represents one of the highest PCE values for cyclopenta[2,1‐b;3,4‐b’]dithiophene (CPDT)‐based OPVs. This polymer is also utilized for constructing semitransparent solar cells and double‐junction tandem solar cells to demonstrate high PCEs of 5.0% and 8.2%, respectively.     

Study of Back Contacts for CdTe Solar Cells

ZnTe/ZnTe:Cu layer is used as a complex back contact.The parmeters of CdTe solar cells with and without the complex back contacts are compared.The effects of un-doped layer thickness,doped concentration and post-deposition annealing temperature of the complex layer on solar cells preformance are investigated.The results show that ZnTe/ZnTe:Cu layer can improve back contacts and largely increase the conversion efficiency of CdTe solar cells.Un-doped layer and post-deposition annealing of high temperature can increase open voltage.Using the complex back contact,a small CdTe cell with fill factor of 73.14% and conversion efficiency of 12.93% is obtained.     

CdS/CdTe太阳电池的背接触

磷硝酸腐蚀是一种适宜于工业化生产的背表面刻蚀工艺.文中采用磷硝酸腐蚀CdTe薄膜,并用溴甲醇腐蚀作为对照实验,研究了两种腐蚀对材料性质的影响.随后用真空蒸发法分别沉积了四种背接触层,提出了适宜于工业化生产的背接触技术,并从实验和理论上对两种背接触结构的CdTe太阳电池进行了分析.     

Morphological Control for High Performance,Solution‐Processed Planar Heterojunction Perovskite Solar Cells

Organometal trihalide perovskite based solar cells have exhibited the highest efficiencies to‐date when incorporated into mesostructured composites. However, thin solid films of a perovskite absorber should be capable of operating at the highest efficiency in a simple planar heterojunction configuration. Here, it is shown that film morphology is a critical issue in planar heterojunction CH₃NH₃PbI_3‐xCl_x solar cells. The morphology is carefully controlled by varying processing conditions, and it is demonstrated that the highest photocurrents are attainable only with the highest perovskite surface coverages. With optimized solution based film formation, power conversion efficiencies of up to 11.4% are achieved, the first report of efficiencies above 10% in fully thin‐film solution processed perovskite solar cells with no mesoporous layer.     

Molecular‐Level Switching of Polymer/Nanocrystal Non‐Covalent Interactions and Application in Hybrid Solar Cells

Hybrid composites obtained upon blending conjugated polymers and colloidal semiconductor nanocrystals are regarded as attractive photo­active materials for optoelectronic applications. Here it is demonstrated that tailoring nanocrystal surface chemistry permits to control non‐covalent and electronic interactions between organic and inorganic components. The pending moieties of organic ligands at the nanocrystal surface are shown to not merely confer colloidal stability while hindering charge separation and transport, but drastically impact morphology of hybrid composites during formation from blend solutions. The relevance of this approach to photovoltaic applications is demonstrated for composites based on poly(3‐hexylthiophene) and lead sulfide nanocrystals, considered as inadequate until this report, which enable the fabrication of hybrid solar cells displaying a power conversion efficiency that reaches 3%. By investigating (quasi)steady‐state and time‐resolved photo‐induced processes in the nanocomposites and their constituents, it is ascertained that electron transfer occurs at the hybrid interface yielding long‐lived separated charge carriers, whereas interfacial hole transfer appears hindered. Here a reliable alternative aiming to gain control over macroscopic optoelectronic properties of polymer/nanocrystal composites by mediating their non‐covalent interactions via ligands' pending moieties is provided, thus opening new possibilities towards efficient solution‐processed hybrid solar cells.     

Solution‐Processed Metal Oxide Nanocrystals as Carrier Transport Layers in Organic and Perovskite Solar Cells

There has been rapid progress in solution‐processed organic solar cells (OSCs) and perovskite solar cells (PVSCs) toward low‐cost and high‐throughput photovoltaic technology. Carrier (electron and hole) transport layers (CTLs) play a critical role in boosting their efficiency and long‐time stability. Solution‐processed metal oxide nanocrystals (SMONCs) as a promising CTL candidate, featuring robust process conditions, low‐cost, tunable optoelectronic properties, and intrinsic stability, offer unique advantages for realizing cost‐effective, high‐performance, large‐area, and mechanically flexible photovoltaic devices. In this review, the recent development of SMONC‐based CTLs in OSCs and PVSCs is summarized. This paper starts with the discussion of synthesis approaches of SMONCs. Then, a broad range of SMONC‐based CTLs, including hole transport layers and electron transport layers, are reviewed, in which an emphasis is placed on the improvement of the efficiency and device stability. Finally, for the better understanding of the challenges and opportunities on SMONC‐based CTLs, several strategies and perspectives are outlined.