A High‐Performance D–A Copolymer Based on Dithieno[3,2‐b:2′,3′‐d]Pyridin‐5(4H)‐One Unit Compatible with Fullerene and Nonfullerene Acceptors in Solar Cells

Development of high‐performance donor–acceptor (D–A) copolymers is vital in the research of polymer solar cells (PSCs). In this work, a low‐bandgap D–A copolymer based on dithieno[3,2‐b:2′,3′‐d]pyridin‐5(4H)‐one unit (DTP), PDTP4TFBT, is developed and used as the donor material for PSCs with PC₇₁BM or ITIC as the acceptor. PDTP4TFBT:PC₇₁BM and PDTP4TFBT:ITIC solar cells give power conversion efficiencies (PCEs) up to 8.75% and 7.58%, respectively. 1,8‐Diiodooctane affects film morphology and device performance for fullerene and nonfullerene solar cells. It inhibits the active materials from forming large domains and improves PCE for PDTP4TFBT:PC₇₁BM cells, while it promotes the aggregation and deteriorates performance for PDTP4TFBT:ITIC cells. The ternary‐blend cells based on PDTP4TFBT:PC₇₁BM:ITIC (1:1.2:0.3) give a decent PCE of 9.20%.     

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.     

Work Function Control of Interfacial Buffer Layers for Efficient and Air‐Stable Inverted Low‐Bandgap Organic Photovoltaics

A water‐soluble cationic polythiophene derivative, poly[3‐(6‐{4‐tert‐butylpyridiniumyl}‐hexyl)thiophene‐2,5‐diyl] [P3(TBP)HT], is combined with anionic poly(3,4‐ethylenedioxythiophene):poly(p‐styrenesulfonate) (PEDOT:PSS) on indium tin oxide (ITO) substrates via electrostatic layer‐by‐layer (eLbL) assembly. By varying the number of eLbL layers, the electrode's work function is precisely controlled from 4.6 to 3.8 eV. These polymeric coatings are used as cathodic interfacial modifiers for inverted‐mode organic photovoltaics that incorporate a photoactive layer composed of either poly[(3‐hexylthiophene)‐2,5‐diyl] (P3HT) and the fullerene acceptor [6,6‐phenyl‐C₆₁‐butyric acid methyl ester (PC₆₁BM) or the low bandgap polymer [poly({4,8‐di(2‐ethylhexyloxyl)benzo[1,2‐b:4,5‐b′]dithiophene}‐2,6‐diyl)‐alt‐({5‐octylthieno[3,4‐c]pyrrole‐4,6‐dione}‐1,3‐diyl) (PBDTTPD)] and the electron acceptor [6,6‐phenyl‐C₇₁‐butyric acid methyl ester (PC₇₁BM)]. The power conversion efficiency (PCE) of the resulting photovoltaic device is dependent on the composition of the eLbL‐assembled interface and permits the fabrication of devices with efficiencies of 3.8% and 5.6% for P3HT and PBDTTPD donor polymers, respectively. Notably, these devices demonstrate significant stability with a P3HT:PC₆₁BM system maintaining 83% of its original PCE after 1 year of storage and a PBDTTPD:PC₇₁BM system maintaining 97% of its original PCE after over 1000 h of storage in air, according to the ISOS‐D‐1 shelf protocol.     

High‐Performance Wide Bandgap Copolymers Using an EDOT Modified Benzodithiophene Donor Block with 10.11% Efficiency

Newly developed benzo[1,2‐b:4,5‐b′]dithiophene (BDT) block with 3,4‐ethylenedioxythiophene (EDOT) side chains is first employed to build efficient photovoltaic copolymers. The resulting copolymers, PBDTEDOT‐BT and PBDTEDOTFBT, have a large bandgap more than 1.80 eV, which is attributed to the increased steric hindrance between the BDT and EDOT skeletons. Both copolymers possess the satisfied absorptions, low‐lying highest occupied molecular orbital (HOMO) levels and high crystallinity. Using the fluorination strategy, PBDTEDOT‐FBT exhibits a wider and stronger absorption and a deeper HOMO level than those of PBDTEDOT‐BT. PBDTEDOT‐FBT:[6,6]‐Phenyl C₇₁ butyric acid methyl ester (PC₇₁BM) blend also shows the higher hole mobility and better surface morphology compared with the PBDTEDOTBT:PC₇₁BM blend. Combination of above advantages, PBDTEDOT‐FBT devices exhibit much higher power conversion efficiency (PCE) of 10.11%, with an improved open circuit voltage (V_oc) of 0.86 V, short circuit current densities (J_sc) of 16.01 mA cm^?2, and fill factor (FF) of 72.6%. This work not only provides a newly efficient candidate of BDT donor block modified with EDOT conjugated side chains, but also achieves high‐performance large bandgap copolymers for polymer solar cells (PSCs) via the synergistic effect of fluorination and side chain engineering strategies.     

Efficient Solution‐Processed Bulk Heterojunction Perovskite Hybrid Solar Cells

Efficient conventional bulk heterojunction (BHJ) perovskite hybrid solar cells (pero‐HSCs) solution‐processed from a composite of CH₃NH₃PbI₃ mixed with PC₆₁BM ([6,6]‐phenyl‐C61‐butyric acid methyl ester), where CH₃NH₃PbI₃ acts as the electron donor and PC₆₁BM acts as the electron acceptor, are reported for the first time. The efficiency of 12.78% is twofold enhancement in comparison with the conventional planar heterojunction pero‐HSCs (6.90%) fabricated by pristine CH₃NH₃PbI₃. The BHJ pero‐HSCs are further optimized by using PC₆₁BM/TiO₂ bi‐electron‐extraction‐layer (EEL), which are both solution‐processed and then followed with low‐temperature thermal annealing. Due to higher electrical conductivity of PC₆₁BM over that of TiO₂, an efficiency of 14.98%, the highest reported efficiency for the pero‐HSCs without incorporating high‐temperature‐processed mesoporous TiO₂ and Al₂O₃ as the EEL and insulating scaffold, is observed from PC₆₁BM modified BHJ pero‐HSCs. Thus, the findings provide a simple way to approach high efficiency low‐cost pero‐HSCs.     

Plasmonic Backscattering Effect in High‐Efficient Organic Photovoltaic Devices

A universal strategy for efficient light trapping through the incorporation of gold nanorods on the electron transport layer (rear) of organic photovoltaic devices is demonstrated. Utilizing the photons that are transmitted through the active layer of a bulk heterojunction photovoltaic device and would otherwise be lost, a significant enhancement in power conversion efficiency (PCE) of poly[N‐9′‐heptadecanyl‐2,7‐carbazole‐alt‐5,5‐(4′,7′‐di‐2‐thienyl‐2′,1′,3′‐benzothiadiazole)]:phenyl‐C₇₁‐butyric acid methyl ester (PCDTBT:PC₇₁BM) and poly[[4,8‐bis[(2‐ethylhexyl)oxy]benzo[1,2‐b:4,5‐b′]dithiophene‐2,6‐diyl][3‐fluoro‐2‐[(2‐ethylhexyl)carbonyl]thieno[3,4‐b] thiophenediyl]] (PTB7):PC₇₁BM by ≈13% and ≈8%, respectively. PCEs over 8% are reported for devices based on the PTB7:PC₇₁BM blend. A comprehensive optical and electrical characterization of our devices to clarify the influence of gold nanorods on exciton generation, dissociation, charge recombination, and transport inside the thin film devices is performed. By correlating the experimental data with detailed numerical simulations, the near‐field and far‐field scattering effects are separated of gold nanorods (Au NRs), and confidently attribute part of the performance enhancement to the enhanced absorption caused by backscattering. While, a secondary contribution from the Au NRs that partially protrude inside the active layer and exhibit strong near‐fields due to localized surface plasmon resonance effects is also observed but is minor in magnitude. Furthermore, another important contribution to the enhanced performance is electrical in nature and comes from the increased charge collection probability.     

A Thieno[3,2‐c]Isoquinolin‐5(4H)‐One Building Block for Efficient Thick‐Film Solar Cells

An aromatic lactam acceptor unit, thieno[3,2‐c]isoquinolin‐5(4H)‐one (TIQ), is developed. Compared with its analogues, dithieno[3,2‐b:2′,3′‐d]pyridin‐5(4H)‐one (DTP) and phenanthridin‐6(5H)‐one (PN), TIQ shows its advantage in constructing donor–acceptor (D–A) copolymers for efficient solar cells. TIQ‐based D–A copolymer PTIQ4TFBT delivers a power conversion efficiency (PCE) of 10.16% in polymer:fullerene solar cells, while those based on DTP and PN copolymers, PDTP4TFBT and PPN4TFBT, afford PCEs around 8.5%. The higher performance of PTIQ4TFBT:PC₇₁BM solar cells originates from enhanced short‐circuit current density (J_sc) and fill factor (FF), because of favorable morphology, less bimolecular recombination, and balanced charge transport in the active layer. Moreover, the performance for PTIQ4TFBT:PC₇₁BM solar cells is less sensitive to active layer thickness than PDTP4TFBT:PC₇₁BM and PPN4TFBT:PC₇₁BM solar cells. Over 8% PCEs can be obtained from PTIQ4TFBT:PC₇₁BM solar cells when the active layer thickness is over 500 nm.     

Side‐Chain Impact on Molecular Orientation of Organic Semiconductor Acceptors: High Performance Nonfullerene Polymer Solar Cells with Thick Active Layer over 400 nm

A new n‐type organic semiconductor (n‐OS) acceptor IDTPC with n‐hexyl side chains is developed. Compared to side chains with 4‐hexylphenyl counterparts (IDTCN), such a design endows the acceptor of IDTPC with higher electron mobility, more ordered face‐on molecular packing, and lower band gap. Therefore, the IDTPC‐based polymer solar cells (PSCs) with a newly developed wide bandgap polymer PTQ10 as donor exhibit the maximum power conversion efficiency (PCE) of 12.2%, a near 65% improvement in PCE relative to the IDTCN‐based control device. Most importantly, the IDTPC‐based device is insensitive to the thickness of the active layer from 70 to 505 nm, which still gives a PCE of 10.0% with the active‐layer thickness of 400 nm. To the best of the authors' knowledge, a PCE of 10.0% is the highest value for the nonfullerene PSCs with an active layer thicker than 400 nm. These results reveal that the blend of PTQ10 and IDTPC exhibits great potential for highly efficient nonfullerene PSCs and large‐area device fabrication.     

High‐Efficiency Polymer Solar Cells Achieved by Doping Plasmonic Metallic Nanoparticles into Dual Charge Selecting Interfacial Layers to Enhance Light Trapping

Significantly increased power conversion efficiency (PCE) of polymer solar cells (PSCs) is achieved by applying a plasmonic enhanced light trapping strategy to a low bandgap conjugated polymer, poly(indacenodithiophene‐ co‐phananthrene‐quinoxaline) (PIDT‐PhanQ) and [6,6]‐phenyl‐C₇₁‐butyric acid methyl ester (PC₇₁BM) based bulk‐heterojunction (BHJ) system. By doping both the rear and front charge‐selecting interfacial layers of the device with different sizes of Au NPs, the PCE of the devices is improved from 6.65% to 7.50% (13% enhancement). A detailed study of processing, characterization, microscopy, and device fabrication is conducted to understand the underlying mechanism for the enhanced device performance. The success of this work provides a simple and generally applicable approach to enhance light harnessing of low bandgap polymers in PSCs.     

Spectral Engineering of Semitransparent Polymer Solar Cells for Greenhouse Applications

In this study, a wavelength selective semitransparent polymer solar cell (ST‐PSC) with a proper transmission spectrum for plant growth is proposed for greenhouse applications. A ternary strategy combining a wide bandgap polymer donor with a near‐infrared absorbing nonfullerene acceptor and a high electron mobility fullerene acceptor is introduced to achieve PSCs with power conversion efficiency (PCE) over 10%. The addition of PC₇₁BM into J52:IEICO‐4F binary blend contributes to the suppressed trap‐assisted recombination, enhanced charge extraction, and improved open‐circuit voltage simultaneously. ST‐PSC based on the J52:IEICO‐4F:PC₇₁BM ternary blend shows an optimized performance with PCE of 7.75% and a defined crop growth factor of 24.8%. Such high‐performance ST‐PSC is achieved by carefully engineering the absorption spectrum of the light harvesting materials. As a result, the transmission spectra of the semitransparent devices are well‐matched with the absorption spectra of the photoreceptors, such as chlorophylls, in green plants, which provides adequate lighting conditions for photosynthesis and plant growth, and therefore making it a competitive candidate for photovoltaic greenhouse applications.     

Study of Burn‐In Loss in Green Solvent‐Processed Ternary Blended Organic Photovoltaics Derived from UV‐Crosslinkable Semiconducting Polymers and Nonfullerene Acceptors

This work deals with the investigation of burn‐in loss in ternary blended organic photovoltaics (OPVs) prepared from a UV‐crosslinkable semiconducting polymer (P2FBTT‐Br) and a nonfullerene acceptor (IEICO‐4F) via a green solvent process. The synthesized P2FBTT‐Br can be crosslinked by UV irradiation for 150 s and dissolved in 2‐methylanisole due to its asymmetric structure. In OPV performance and burn‐in loss tests performed at 75 °C or AM 1.5G Sun illumination for 90 h, UV‐crosslinked devices with PC₇₁BM show 9.2% power conversion efficiency (PCE) and better stability against burn‐in loss than pristine devices. The frozen morphology resulting from the crosslinking prevents lateral crystallization and aggregation related to morphological degradation. When IEICO‐4F is introduced in place of a fullerene‐based acceptor, the burn‐in loss due to thermal aging and light soaking is dramatically suppressed because of the frozen morphology and high miscibility of the nonfullerene acceptor (18.7% → 90.8% after 90 h at 75 °C and 37.9% → 77.5% after 90 h at AM 1.5G). The resulting crosslinked device shows 9.4% PCE (9.8% in chlorobenzene), which is the highest value reported to date for crosslinked active materials, in the first green processing approach.     

Self‐Organization of Polymer Additive,Poly(2‐vinylpyridine) via One‐Step Solution Processing to Enhance the Efficiency and Stability of Polymer Solar Cells

Interfaces between the photoactive layers and electrodes play critical roles in controlling the performance of optoelectronic devices. Herein, a novel nonconjugated polymer additive (nPA), poly(2‐vinylpyridine) (P2VP), is reported for modifying the interfaces between the bulk‐heterojunction (BHJ) and cathode/metal oxide (MO) layers. The P2VP nPA enables remarkably enhanced power conversion efficiencies (PCEs) and ambient stability in different types of polymer solar cells (PSCs). Importantly, interfacial engineering can be achieved during deposition of the P2VP nPA‐containing BHJ active layer via simple, one‐step solution processing. The P2VP nPA has much higher surface energy than the BHJ active components and stronger interaction with the surface of MO, which affords spontaneous vertical phase separation from the BHJ layer on the MO surface by one‐step solution processing. The self‐assembled P2VP layer substantially reduces the work function and surface defect density of MO, thereby minimizing the charge‐extraction barrier and increasing the PCEs of the PSCs significantly, i.e., PTB7‐Th:PC₇₁BM (10.53%→11.14%), PTB7:PC₇₁BM (7.37%→8.67%), and PTB7‐Th:P(NDI2HD‐T) all‐PSCs (5.52%→6.14%). In addition, the lifetimes of the PSCs are greatly improved by the use of the P2VP nPA.     

Efficiency Enhancement of Polymer Solar Cells Based on Poly(3‐hexylthiophene)/Indene‐C70 Bisadduct via Methylthiophene Additive

Photovoltaic performance of polymer solar cells based on poly(3‐hexylthiophene) (P3HT) as the donor and indene‐C₇₀ bisadduct (IC₇₀BA) as the acceptor is improved by adding 3 vol% 3‐methylthiophene (MT) or 3‐hexylthiophene (HT) as processing additives. The results of UV‐vis absorption spectroscopy, X‐ray diffraction analysis and atomic force microscopy indicate that with the MT or HT processing additive, the active layer of the blend of P3HT/IC₇₀BA showed strengthened absorbance, enhanced crystallinity and improved film morphology. The power conversion efficiency (PCE) of the PSCs was improved from 5.80% for the device without the additive to 6.35% for the device with HT additive and to 6.69% with MT additive. The PCE of 6.69% is the top value reported so far for the PSCs based on P3HT.     

Significantly Enhancing the Efficiency of a New Light‐Harvesting Polymer with Alkylthio naphthyl Substituents Compared to Their Alkoxyl Analogs

In this work, a new benzo[1,2‐b:4,5‐b′]dithiophene (BDT) building block containing alkylthio naphthyl as a side chain is designed and synthesized, and the resulting polymer, namely PBDTNS‐BDD, shows a lower HOMO energy level than that of its alkoxyl naphthyl counterpart PBDTNO‐BDD. An optimized photovoltaic device using PBDTNS‐BDD as a donor exhibits power conversion efficiencies (PCE) of 8.70% and 9.28% with the fullerene derivative PC₇₁BM and the fullerene‐free small molecule ITIC as acceptors, respectively. Surprisingly, ternary blend devices based on PBDTNS‐BDD and two acceptors, namely PC₇₁BM and ITIC, shows a PCE of 11.21%, which is much higher than that of PBDTNO‐BDD based ternary devices (7.85%) even under optimized conditions.     

Impact of Fullerene Molecular Weight on P3HT:PCBM Microstructure Studied Using Organic Thin‐Film Transistors

The clustering and diffusion of C₇₁‐butyric acid methyl ester (PC₇₁BM) in poly(3‐hexylthiophene) (P3HT) has been studied using single layer blend and bilayer organic field‐effect transistors (OFETs) and by atomic force microscopy (AFM). P3HT:PC₇₁BM blend based OFETs were found to undergo phase‐segregation upon annealing, which was detectable as a fall in electron mobility with increasing annealing temperature. By employing carefully designed bilayer P3HT:PC₇₁BM OFETs, the diffusion‐properties of PC₇₁BM in P3HT could additionally be inferred from electron mobility measurements. It was found that the prerequisite annealing temperatures for detectable PC₇₁BM clustering and diffusion in P3HT was approximately 20 °C higher than for PC₆₁BM. The diffusion coefficient of PC₆₁BM in P3HT was found to be several times higher that that of PC₇₁BM. The present work provides unique insights into the diffusion process of fullerenes in conjugated polymers and could prove highly valuable for future materials development and device optimization.     

Plasmon‐Enhanced Polymer Photovoltaic Device Performance Using Different Patterned Ag/PVP Electrospun Nanofibers

Significant enhancement of P3HT (poly(3‐hexylthiophene)):PC₆₁BM ([6,6]‐phenyl C61‐butyric acid methyl ester) photovoltaic devices using different patterns of electrospun Ag/PVP composite nanofibers, including nonwoven, aligned, and crossed patterns, is reported. The composite electrospun nanofibers are prepared using in situ reduction of silver (Ag) nanoparticles in Ag/poly(vinyl pyrrolidone) (PVP) via a two‐fluid coaxial electrospinning technique. The composition, crystalline orientation, and particle size of Ag are manipulated by controlling the core/shell solution concentration. The smallest diameter of the composite nanofibers leads to the highest orientation of the Ag nanoparticles and results in the largest conductivity due to geometric confinement. Such composite nanofibers exhibit the surface plasmon resonance (SPR) effect, which provides near field enhancement of electromagnetic field around active layer. Additionally, composite nanofibers with the crossed or nonwoven patterns further enhance high carrier mobility, compared to that of the aligned pattern. It leads to the 18.7% enhancement of the power conversion efficiency of photovoltaic cell compared to the parent device. The results indicate that the high conductivity and SPR effect of the Ag/PVP electrospun nanofibers can significantly improve the photocurrent and PCE, leading to promising organic solar cell applications.     

8.0% Efficient All‐Polymer Solar Cells with High Photovoltage of 1.1 V and Internal Quantum Efficiency near Unity

In very recent years, growing efforts have been devoted to the development of all‐polymer solar cells (all‐PSCs). One of the advantages of all‐PSCs over the fullerene‐based PSCs is the versatile design of both donor and acceptor polymers which allows the optimization of energy levels to maximize the open‐circuit voltage (V_oc). However, there is no successful example of all‐PSCs with both high V_oc over 1 V and high power conversion efficiency (PCE) up to 8% reported so far. In this work, a combination of a donor polymer poly[4,8‐bis(5‐(2‐octylthio)thiophen‐2‐yl)benzo[1,2‐b:4,5‐b′]dithiophene‐2,6‐diyl‐alt‐(5‐(2‐ethylhexyl)‐4H‐thieno[3,4‐c]pyrrole‐4,6(5H)‐dione)‐1,3‐diyl] (PBDTS‐TPD) with a low‐lying highest occupied molecular orbital level and an acceptor polymer poly[[N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐thiophene‐2,5‐diyl] (PNDI‐T) with a high‐lying lowest unoccupied molecular orbital level is used, realizing high‐performance all‐PSCs with simultaneously high V_oc of 1.1 V and high PCE of 8.0%, and surpassing the performance of the corresponding PC₇₁BM‐based PSCs. The PBDTS‐TPD:PNDI‐T all‐PSCs achieve a maximum internal quantum efficiency of 95% at 450 nm, which reveals that almost all the absorbed photons can be converted into free charges and collected by electrodes. This work demonstrates the advantages of all‐PSCs by incorporating proper donor and acceptor polymers to boost both V_oc and PCEs.     

Structural Characterization of a Composition Tolerant Bulk Heterojunction Blend

The ratio of the donor and acceptor components in bulk heterojunction (BHJ) organic solar cells is a key parameter for achieving optimal power conversion efficiency (PCE). However, it has been recently found that a few BHJ blends have compositional tolerance and achieve high performance in a wide range of donor to acceptor ratios. For instance, the X2 :PC₆₁BM system, where X2 is a molecular donor of intermediate dimensions, exhibits a PCE of 6.6%. Its PCE is relatively insensitive to the blend ratio over the range from 7:3 to 4:6. The effect of blend ratio of X2 /PC₆₁BM on morphology and device performance is therefore systematically investigated by using the structural characterization techniques of energy‐filtered transmission energy microscopy (EF‐TEM), resonant soft X‐ray scattering (R‐SoXS) and grazing incidence wide angle X‐ray scattering (GIWAXS). Changes in blend ratio do not lead to obvious differences in morphology, as revealed by R‐SoXS and EF‐TEM. Rather, there is a smooth evolution of a connected structure with decreasing domain spacing from 8:2 to 6:4 blend ratios. Domain spacing remains constant from 6:4 to 4:6 blend ratios, which suggests the presence of continuous phases with proper domain size that may provide access for charge carriers to reach their corresponding electrodes.     

Synergic Interface and Optical Engineering for High‐Performance Semitransparent Polymer Solar Cells

In this study the thickness of the PTB7‐Th:PC₇₁BM bulk heterojunction (BHJ) film and the PF3N‐2TNDI electron transport layer (ETL) is systematically tuned to achieve polymer solar cells (PSCs) with optimized power conversion efficiency (PCE) of over 9% when an ultrathin BHJ of 50 nm is used. Optical modeling suggests that the high PCE is attributed to the optical spacer effect from the ETL, which not only maximizes the optical field within the BHJ film but also facilitates the formation of a more homogeneously distributed charge generation profile across the BHJ film. Experimentally it is further proved that the extra photocurrent produced at the PTB7‐Th/PF3N‐2TNDI interface also contributes to the improved performance. Taking advantage of this high performance thin film device structure, one step further is taken to fabricate semitransparent PSCs (ST‐PSCs) by using an ultrathin transparent Ag cathode to replace the thick Ag mirror cathode, yielding a series of high performance ST‐PSCs with PCEs over 6% and average visible transmittance between 20% and 30%. These ST‐PSCs also possess remarkable transparency color perception and rendering properties, which are state‐of‐the‐art and fulfill the performance criteria for potential use as power‐generating windows in near future.     

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.