Physically Stable Polymer‐Membrane Electrolytes for Highly Efficient Solid‐State Dye‐Sensitized Solar Cells with Long‐Term Stability

A 3D polymer‐network‐membrane (3D‐PNM) electrolyte is described for highly stable, solid‐state dye‐sensitized solar cells (DSCs) with excellent power‐conversion efficiency (PCE). The 3D‐PNM electrolyte is prepared by using one‐pot in situ cross‐linking polymerization on the surface of dye‐sensitized TiO₂ particles in the presence of redox species. This method allows the direct connection of the 3D‐PNM to the surface of the TiO₂ particles as well as the in situ preparation of the electrolyte gel during device assembly. There are two junction areas (liquid and solid‐state junctions) in the DSCs that employ conventional polymer electrolytes, and the major interface is at the liquid‐state junction. The solid‐state junction is dominant in the DSCs that employ the 3D‐PNM electrolyte, which exhibit almost constant performance during aging at 65 °C for over 700 h (17.0 to 17.2 mA cm^–2). The best cell performance gives a PCE of 9.1%; this is slightly better than the performance of a DSC that employs a liquid electrolyte.     

Fully Plastic Dye Solar Cell Devices by Low‐Temperature UV‐Irradiation of both the Mesoporous TiO2 Photo‐ and Platinized Counter‐Electrodes

The application of UV irradiation processes are successfully proposed for the first time in the fabrication of both of the two plastic electrodes in flexible dye solar cells (DSCs) and modules. For the realization of the photo‐electrode, a customized TiO₂ paste formulation and UV processing method was developed which yields 134% (48%) performance enhancement with respect to the same (binder‐free) paste treated at 120 °C. UV treatment induces both complete removal of organic media and more efficient charge collection. Significantly, highly catalytic platinized flexible counter‐electrodes are also obtained via UV photo‐induced reduction of screen‐printed platinum precursor pastes based on hexachloroplatinic acid. Using both UV‐processed electrodes, a fully plastic DSC is fabricated with a conversion efficiency of 4.3% under 1 Sun (semitransparent) and 5.3% under 0.2 Sun (opaque). Performance is within 10% of the efficiency of a glass‐based DSC prepared with the same materials but with conventional high temperature processes. The material formulations and processes are simple, and easily up‐scaled over large areas, even directly and simultaneously applicable to the preparation of both the photo‐and counter‐electrode on the same substrate which enabled us to demonstrate the first module on plastic realized with a W series interconnection.     

The Role of Antireflective Coating CYTOP,Immersion Oil,and Sensitizer Selection in Fabricating a 2.3 V, 10% Power Conversion Efficiency SSM‐DSC Device

Sequential series multijunction dye‐sensitized solar cells (SSM‐DSCs) can power solar‐to‐fuel processes with a single illuminated area device. Dye selection and strategies limiting photon losses are critical in SSM‐DSC devices for higher performance systems. Herein, an efficient and readily applicable spin coating protocol on glass surfaces with an antireflective fluoropolymer (CYTOP) is applied to an SSM‐DSC architecture. Combining CYTOP with the use of an immersion oil between glass spacers in a three subcell SSM‐DSC with judiciously selected TiO₂ photoanode sensitizers and thicknesses, an overall power conversion efficiency (PCE) of 10.1% is obtained with an output of 2.3 V. Without external bias, this SSM‐DSC configuration shows an impressive overall solar‐to‐fuel conversion efficiency of 6% when powering IrO₂ and Au₂O₃ electrocatalysts for CO₂ and H₂O to CO and H₂ conversion in aqueous solution. The role of CYTOP, immersion oil, sensitizer selection, and film thickness on SSM‐DSC devices is discussed along with the stability of this system.     

TiO2 Nanocrystals Synthesized by Laser Pyrolysis for the Up‐Scaling of Efficient Solid‐State Dye‐Sensitized Solar Cells

A crucial issue regarding emerging nanotechnologies remains the up‐scaling of new functional nanostructured materials towards their implementation in high performance applications on a large scale. In this context, we demonstrate high efficiency solid‐state dye‐sensitized solar cells prepared from new porous TiO₂ photoanodes based on laser pyrolysis nanocrystals. This strategy exploits a reduced number of processing steps as well as non‐toxic chemical compounds to demonstrate highly porous TiO₂ films. The possibility to easily tune the TiO₂ nanocrystal physical properties allows us to demonstrate all solid‐state dye‐sensitized devices based on a commercial benchmark materials (organic indoline dye and molecular hole transporter) presenting state‐of‐the‐art performance comparable with reference devices based on a commercial TiO₂ paste. In particular, a drastic improvement in pore infiltration, which is found to balance a relatively lower surface area compared to the reference electrode, is evidenced using laser‐synthesized nanocrystals resulting in an improved short‐circuit current density under full sunlight. Transient photovoltage decay measurements suggest that charge recombination kinetics still limit device performance. However, the proposed strategy emphasizes the potentialities of the laser pyrolysis technique for up‐scaling nanoporous TiO₂ electrodes for various applications, especially for solar energy conversion.     

Titanium Dioxide Mesoporous Electrodes for Solid‐State Dye‐Sensitized Solar Cells: Cross‐Analysis of the Critical Parameters

We report a comparative study on the use of four different mesoporous titanium dioxide (TiO₂) photo‐electrodes for the fabrication of solid‐state dye‐sensitized solar cells (sDSSCs). The photovoltaic parameters of the device correlate with several intrinsic properties of the film, based not only on its morphological features, as commonly considered in standard characterizations, but also on the transport and the electronic properties of the photo‐electrode. These properties differ significantly for TiO₂ electrodes processed using different colloidal pastes, and are decisive for the photovoltaic efficiency, ranging from 3.7% up to 5.1%. In particular, the dielectric permittivity of each mesoporous layer (ε_eff) and the number of traps (N_t) determined by the space‐charge‐limited current (SCLC) theory are found to be a bottle‐neck for the charge transport, greatly influencing the fill factor (FF) and open circuit voltage (V_oc) of the cells. In addition, a direct correlation between TiO₂ surface potential with the V_oc was established. Cross‐analysis of key macroscopic parameters of the films prior to integration in the devices, in particular focusing on the determination of the capacitance and surface potential shift of the TiO₂ mesoporous anode, represents a straightforward yet powerful method to screen and select the most suitable TiO₂ for applications in sDSSCs.     

Molecularly Engineered Phthalocyanines as Hole‐Transporting Materials in Perovskite Solar Cells Reaching Power Conversion Efficiency of 17.5%

Easily accessible tetra‐5‐hexylthiophene‐, tetra‐5‐hexyl‐2,2′‐bisthiophene‐substituted zinc phthalocyanines (ZnPcs) and tetra‐tert ‐butyl ZnPc are employed as hole‐transporting materials in mixed‐ion perovskite [HC(NH₂)₂]_0.85(CH₃NH₃)_0.15Pb(I_0.85Br_0.15)₃ solar cells, reaching the highest power conversion efficiency (PCE) so far for phthalocyanines. Results confirm that the photovoltaic performance is strongly influenced by both, the individual optoelectronic properties of ZnPcs and the aggregation of these tetrapyrrolic semiconductors in the solid thin film. The optimized devices exhibit PCE of 15.5% when using tetra‐5‐hexyl‐2,2′‐bisthiophene substituted ZnPcs, 13.3% for tetra‐tert ‐butyl ZnPc, and a record 17.5% for tetra‐5‐hexylthiophene‐based analogue under standard global 100 mW cm^?2 AM 1.5G illumination. These results boost up the potential of solution‐processed ZnPc derivatives as stable and economic hole‐transport materials for large‐scale applications, opening new frontiers toward a realistic, efficient, and inexpensive energy production.     

Overcoming Interfacial Losses in Solution‐Processed Organic Multi‐Junction Solar Cells

Organic solar cells are promising in terms of full‐solution‐processing which enables low‐cost and large‐scale fabrication. While single‐junction solar cells have seen a boost in power conversion efficiency (PCE), multi‐junction solar cells are promising to further enhance the PCE. In all‐solution‐processed multi‐junction solar cells, interfacial losses are often encountered between hole‐transporting layer (HTL) and the active layers and therefore greatly limit the application of newly developed high‐performance donor and acceptor materials in multi‐junction solar cells. Here, the authors report on a systematic study of interface losses in both single‐junction and multi‐junction solar cells based on representative polymer donors and HTLs using electron spectroscopy and time‐of‐flight secondary ion mass spectrometry. It is found that a facile mixed HTL containing poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and MoO _x nanoparticles successfully overcomes the interfacial losses in both single‐ and multi‐junction solar cells based on various active layers by reducing interface protonation, promoting better energy‐level alignment, and forming a dense and smooth layer. Solution‐processed single‐junction solar cells are demonstrated to reach the same performance as with evaporated MoO _x (over 7%). Multi‐junction solar cells with polymers containing nitrogen atoms as the first layer and the mixed PEDOT:PSS and MoO _x nanoparticles as hole extraction layer reach fill factor (FF) of over 60%, and PCE of over 8%, while the identical stack with pristine PEDOT:PSS or MoO _x nanoparticles show FF smaller than 50% and PCE less than 5%.     

Surface Engineering of TiO2 ETL for Highly Efficient and Hysteresis‐Less Planar Perovskite Solar Cell (21.4%) with Enhanced Open‐Circuit Voltage and Stability

Interfacial studies and band alignment engineering on the electron transport layer (ETL) play a key role for fabrication of high‐performance perovskite solar cells (PSCs). Here, an amorphous layer of SnO₂ (a‐SnO₂) between the TiO₂ ETL and the perovskite absorber is inserted and the charge transport properties of the device are studied. The double‐layer structure of TiO₂ compact layer (c‐TiO₂) and a‐SnO₂ ETL leads to modification of interface energetics, resulting in improved charge collection and decreased carrier recombination in PSCs. The optimized device based on a‐SnO₂/c‐TiO₂ ETL shows a maximum power conversion efficiency (PCE) of 21.4% as compared to 19.33% for c‐TiO₂ based device. Moreover, the modified device demonstrates a maximum open‐circuit voltage (V_oc) of 1.223 V with 387 mV loss in potential, which is among the highest reported value for PSCs with negligible hysteresis. The stability results show that the device on c‐TiO₂/a‐SnO₂ retains about 91% of its initial PCE value after 500 h light illumination, which is higher than pure c‐TiO₂ (67%) based devices. Interestingly, using a‐SnO₂/c‐TiO₂ ETL the PCE loss was only 10% of initial value under continuous UV light illumination after 30 h, which is higher than that of c‐TiO₂ based device (28% PCE loss).     

Slot‐Die and Roll‐to‐Roll Processed Single Junction Organic Photovoltaic Cells with the Highest Efficiency

The record efficiency of the state‐of‐the‐art polymer solar cells (PSCs) is rapidly increasing, due to the discovery of high‐performance photoactive donor and acceptor materials. However, strong questions remain as to whether such high‐efficiency PSCs can be produced by scalable processes. This paper reports a high power conversion efficiency (PCE) of 13.5% achieved with single‐junction ternary PSCs based on PTB7‐Th, PC₇₁BM, and COi8DFIC fabricated by slot‐die coating, which shows the highest PCE ever reported in PSCs fabricated by a scalable process. To understand the origin of the high performance of the slot‐die coated device, slot‐die coated photoactive films and devices are systematically investigated. These results indicate that the good performance of the slot‐die PSCs can be due to a favorable molecule‐structure and film‐morphology change by introducing 1,8‐diiodooctane and heat treatment, which can lead to improved charge transport with reduced carrier recombination. The optimized condition is then used for the fabrication of large‐area modules and also for roll‐to‐roll fabrication. The slot‐die coated module with 30 cm² active‐area and roll‐to‐roll produced flexible PSC has shown 8.6% and 9.6%, respectively. These efficiencies are the highest in each category and demonstrate the strong potential of the slot‐die coated ternary system for commercial applications.     

Vacuum‐Assisted Growth of Low‐Bandgap Thin Films (FA0.8MA0.2Sn0.5Pb0.5I3) for All‐Perovskite Tandem Solar Cells

All‐perovskite multijunction photovoltaics, combining a wide‐bandgap (WBG) perovskite top solar cell (E_G ≈1.6–1.8 eV) with a low‐bandgap (LBG) perovskite bottom solar cell (E_G < 1.3 eV), promise power conversion efficiencies (PCEs) >33%. While the research on WBG perovskite solar cells has advanced rapidly over the past decade, LBG perovskite solar cells lack PCE as well as stability. In this work, vacuum‐assisted growth control (VAGC) of solution‐processed LBG perovskite thin films based on mixed Sn–Pb perovskite compositions is reported. The reported perovskite thin films processed by VAGC exhibit large columnar crystals. Compared to the well‐established processing of LBG perovskites via antisolvent deposition, the VAGC approach results in a significantly enhanced charge‐carrier lifetime. The improved optoelectronic characteristics enable high‐performance LBG perovskite solar cells (1.27 eV) with PCEs up to 18.2% as well as very efficient four‐terminal all‐perovskite tandem solar cells with PCEs up to 23%. Moreover, VAGC leads to promising reproducibility and potential in the fabrication of larger active‐area solar cells up to 1 cm².     

Ionic Liquid–Sulfolane Composite Electrolytes for High‐Performance and Stable Dye‐Sensitized Solar Cells

Ionic liquid electrolytes are prepared using sulfolane as a plasticizer for eutectic melts to realize highly stable and efficiently performing dye‐sensitized solar cells (DSCs) in hot climate conditions. Variations in the viscosity of the formulations with sulfolane content are measured and performance in DSCs is investigated using the ruthenium dye C106 as a sensitizer. A power conversion efficiency (PCE) of 8.2% is achieved under standard reporting conditions. Apart from lowering the viscosity, the addition of sulfolane induces a negative shift of the TiO₂ conduction band edge. Strikingly the device performance increases to 8.4% at 50 °C due to higher short circuit photocurrent and fill factor, over‐compensating the loss in open circuit voltage with increasing temperature. The PCE increases also upon decreasing the light intensity of the solar simulator, reaching up to 9% at 50 mW cm^?2. Devices based on these new electrolyte formulations show excellent stability during light soaking for 2320 h under full sunlight at 60 °C and also during a 1065 h long heat stress at 80 °C in the dark. A detailed investigation provides important information about the factors affecting the principal photovoltaic parameters during the aging process and the first results from a series of outdoor measurements are reported.     

Highly stable and Efficient Perovskite Solar Cells Based on FAMA‐Perovskite‐Cu:NiO Composites with 20.7% Efficiency and 80.5% Fill Factor

To solve critical issues related to device stability and performance of perovskite solar cells (PSCs), FA_0.026MA_0.974PbI_3?yCl_y‐Cu:NiO (formamidinium methylammonium (FAMA)‐perovskite‐Cu:NiO) and Al₂O₃/Cu:NiO composites are developed and utilized for fabrication of highly stable and efficient PSCs through fully‐ambient‐air processes. The FAMA‐perovskite‐Cu:NiO composite crystals prepared without using any antisolvents not only improve the perovskite film quality with large‐size crystals and less grain boundaries but also tailor optical and electronic properties and suppress charge recombination with reduction of trap density. A champion device based on the composites as light absorber and Al₂O₃/Cu:NiO interfacial layer between electron transport layer and active layer yields power conversion efficiency (PCE) of 20.67% with V_OC of 1.047 V, J_SC of 24.51 mA cm^?2, and fill factor of 80.54%. More importantly, such composite‐based PSCs without encapsulation show significant enhancement in long‐term air‐stability, thermal‐ and photostability with retaining 97% of PCE over 240 d under ambient conditions (25–30 °C, 45–55% humidity).     

New Strategy for Two‐Step Sequential Deposition: Incorporation of Hydrophilic Fullerene in Second Precursor for High‐Performance p‐i‐n Planar Perovskite Solar Cells

In p‐i‐n planar perovskite solar cells (pero‐SCs) based on methylammonium lead iodide (MAPbI₃) perovskite, high‐quality MAPbI₃ film, perfect interfacial band alignment and efficient charge extracting ability are critical for high photovoltaic performance. In this work, a hydrophilic fullerene derivative [6,6]‐phenyl‐C₆₁‐butyric acid‐(3,4,5‐tris(2‐(2‐(2‐methoxyethoxy)ethoxy)ethoxy)phenyl)methanol ester (PCBB‐OEG) is introduced as additive in the methylammonium iodide precursor solution in the preparation of MAPbI₃ perovskite film by two‐step sequential deposition method, and obtained a top‐down gradient distribution with an ultrathin top layer of PCBB‐OEG. Meanwhile, a high‐quality perovskite film with high crystallinity, less trap‐states, and dense‐grained uniform morphology can well grow on both hydrophilic (poly(3,4‐ethylenedioxythiophene)/poly(styrenesulfonic acid)) and hydrophobic (polytriarylamine, PTAA) hole transport layers. When the PCBB‐OEG‐containing perovskite film (pero‐0.1) is prepared in a p‐i‐n planar pero‐SC with the configuration of ITO/PTAA/pero‐0.1/[6,6]‐phenyl‐C₆₁‐butyric acid methyl ester/Al, the device delivers a promising power conversion efficiency (PCE) of 20.2% without hysteresis, which is one of the few PCE over 20% for the p‐i‐n planar pero‐SCs. Importantly, the pero‐0.1‐based device shows an excellent stability that can retain 98.4% of its initial PCE after being exposed for 300 h under ambient atmosphere with a high humidity, and the flexible pero‐SCs based on pero‐0.1 also demonstrate a promising PCE of 18.1%.     

Transforming Benzophenoxazine Laser Dyes into Chromophores for Dye‐Sensitized Solar Cells: A Molecular Engineering Approach

The refunctionalization of a series of four well‐known industrial laser dyes, based on benzophenoxazine, is explored with the prospect of molecularly engineering new chromophores for dye‐sensitized solar cell (DSC) applications. Such engineering is important since a lack of suitable dyes is stifling the progress of DSC technology. The conceptual idea involves making laser dyes DSC‐active by chemical modification, while maintaining their key property attributes that are attractive to DSC applications. This molecular engineering follows a stepwise approach. First, molecular structures and optical absorption properties are determined for the parent laser dyes: Cresyl Violet ( 1 ), Oxazine 170 ( 2 ), Nile Blue A ( 3 ), Oxazine 750 ( 4 ). These reveal structure‐property relationships which define the prerequisites for computational molecular design of DSC dyes; the nature of their molecular architecture (D‐π‐A) and intramolecular charge transfer. Second, new DSC dyes are computationally designed by the in silico addition of a carboxylic acid anchor at various chemical substitution points in the parent laser dyes. A comparison of the resulting frontier molecular orbital energy levels with the conduction band edge of a TiO₂ DSC photoanode and the redox potential of two electrolyte options I^?/I₃^? and Co^(II/III)tris(bipyridyl) suggests promise for these computationally designed dyes as co‐sensitizers for DSC applications.     

Layer‐by‐Layer Solution‐Processed Low‐Bandgap Polymer‐PC61BM Solar Cells with High Efficiency

Polymer solar cells (PSCs) are fabricated without solvent additives using a low‐bandgap polymer, PBDTTT‐C‐T, as the donor and [6,6]‐phenyl‐C61‐butyric‐acid‐methyl‐ester (PC₆₁BM) as the acceptor. Donor‐acceptor blend and layer‐by‐layer (LL) solution process are used to form active layers. Relative to the blend devices, the LL devices exhibit stronger absorption, better vertical phase separation, higher hole and electron mobilities, and better charge extraction at correct electrodes. As a result, after thermal annealing the LL devices exhibit an average power conversion efficiency (PCE) of 6.86%, which is much higher than that of the blend devices (4.31%). The best PCE of the LL devices is 7.13%, which is the highest reported for LL processed PSCs and among the highest reported for PC₆₁BM‐based single‐junction PSCs.     

Solution‐Processed TiO2 Nanoparticles as the Window Layer for CuIn(S,Se)2 Devices

As a wide‐bandgap semiconductor, titanium dioxide (TiO₂) with a porous structure has proven useful in dye‐sensitized solar cells, but its application in low‐cost, high‐efficiency inorganic photovoltaic devices based on materials such as Cu(InGa)Se₂ or Cu₂ZnSnS₄ is limited. Here, a thin film made from solution‐processed TiO₂ nanocrystals is demonstrated as an alternative to intrinsic zinc oxide (i‐ZnO) as the window layer of CuInS_xSe_1?x solar cells. The as‐synthesized, well‐dispersed, 6 nm TiO₂ nanocrystals are assembled into thin films with controllable thicknesses of 40, 80, and 160 nm. The TiO₂ nanocrystal films with thicknesses of 40 and 80 nm exhibit conversion efficiencies (6.2% and 6.33%, respectively) that are comparable to that of a layer of the typical sputtered i‐ZnO (6.42%). The conversion efficiency of the devices with a TiO₂ thickness of 160 nm decreases to 2.2%, owing to the large series resistance. A 9‐hour reaction time leads to aggregated nanoparticles with a much‐lower efficiency (2%) than that of the well‐dispersed TiO₂ nanoparticles prepared using a 15‐hour reaction time. Under optimized conditions, the champion TiO₂ nanocrystal‐film‐based device shows even higher efficiency (9.2%) than a control device employing a typical i‐ZnO film (8.6%).     

High‐Performance Small Molecule via Tailoring Intermolecular Interactions and its Application in Large‐Area Organic Photovoltaic Modules

Solution‐processed organic solar cells are promising owing to their light weight, ease of processability, low cost, flexibility, and large‐area fabrication. Particularly, small‐molecule active materials have been recently developed using straightforward synthesizing methods, exhibiting the least batch‐to‐batch variation in physical and optoelectronic properties and highly reproducible efficiency. A series of 2D‐BDT‐based active materials with various numbers of benzodithiophene (BDT) units and how the number of 2D‐BDT units influences the construction of a well‐defined interconnected structure are reported. The systematically controlled morphology of the 2D‐BDT material helps achieve a high power‐conversion efficiency (PCE) of 8.56% and a high fill factor of 0.73 without the use of additives. The reduced charge recombination and well‐constructed morphology of this material facilitate a PCE of 7.45% in a 77.8 cm² rigid module, which is the outstanding performance in large‐area modules.     

Green‐Solvent‐Processed All‐Polymer Solar Cells Containing a Perylene Diimide‐Based Acceptor with an Efficiency over 6.5%

To realize high power conversion efficiencies (PCEs) in green‐solvent‐processed all‐polymer solar cells (All‐PSCs), a long alkyl chain modified perylene diimide (PDI)‐based polymer acceptor PPDIODT with superior solubility in nonhalogenated solvents is synthesized. A properly matched PBDT‐TS1 is selected as the polymer donor due to the red‐shifted light absorption and low‐lying energy level in order to achieve the complementary absorption spectrum and matched energy level between polymer donor and polymer acceptor. By utilizing anisole as the processing solvent, an optimal efficiency of 5.43% is realized in PBDT‐TS1/PPDIODT‐based All‐PSC with conventional configuration, which is comparable with that of All‐PSCs processed by the widely used binary solvent. Due to the utilization of an inverted device configuration, the PCE is further increased to over 6.5% efficiency. Notably, the best‐performing PCE of 6.58% is the highest value for All‐PSCs employing PDI‐based polymer acceptors and green‐solvent‐processed All‐PSCs. The excellent photovoltaic performance is mainly attributed to a favorable vertical phase distribution, a higher exciton dissociation efficiency (P_diss) in the blend film, and a higher electrode carrier collection efficiency. Overall, the combination of rational molecular designing, material selection, and device engineering will motivate the efficiency breakthrough in green‐solvent‐processed All‐PSCs.     

Dominating Energy Losses in NiO p‐Type Dye‐Sensitized Solar Cells

Nickel oxide based p‐type dye‐sensitized solar cells (DSCs) are limited in their efficiencies by poor fill factors (FFs). This work explores the origins of this limitation. Transient absorption spectroscopy identifies fast recombination between the injected hole and the dye anion under applied load as one of the predominant reasons for the poor FF of NiO‐based DSCs. A reduced hole injection efficiency, η_INJ, under applied load is found to play an equally important role. Both, the dye regeneration yield, Φ_REG, and η_INJ decrease by approximately 40%–50% when moving from short‐ to open‐circuit conditions. Spectroelectrochemical measurements reveal that the electrochromic properties of NiO are a further limiting factor for the device performance leading to variable light‐harvesting efficiencies, η_LH, under applied load. The peak light‐harvesting efficiency decreases from 63% at short circuit to 57% at 600 mV reducing the FF of NiO DSCs by 5%. This effect is expected to be more pronounced for future devices with higher operating voltages. Incident, photon‐to‐electron conversion efficiency front–back analysis at applied bias is utilized to characterize the interfacial charge recombination. It is found that the recombination between the injected hole and the redox mediator has a surprisingly small effect on the FF.     

In‐situ Crosslinking and n‐Doping of Semiconducting Polymers and Their Application as Efficient Electron‐Transporting Materials in Inverted Polymer Solar Cells

In this study, we demonstrate in‐situ n‐doping and crosslinking of semiconducting polymers as efficient electron‐transporting materials for inverted configuration polymer solar cells. The semiconducting polymers were crosslinked with bis(perfluorophenyl) azide (bis‐PFPA) to form a robust solvent‐resistant film, thereby preventing solvent‐induced erosion during subsequent solution‐based device processing. In addition, chemical n‐doping of semiconducting polymers with (4‐(1,3‐dimethyl‐2,3‐dihydro‐1H‐benzoimidazol‐2‐yl)phenyl)dimethylamine (N‐DMBI) substantially improved the power conversion efficiency of solar cells from 0.69% to 3.42%. These results open the way for progress on generally applicable polymeric interface materials, providing not only high device performance but also an effective fabrication method for solution‐processed multilayer solar cell devices.