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Indoor photovoltaics (IPVs) are garnering increasing attention from both the academic and industrial communities due to the pressing demand of the ecosystem of Internet-of-Things. All-polymer solar cells (all-PSCs), emerging as a sub-type of organic photovoltaics, with the merits of great film-forming properties, remarkable morphological and light stability, hold great promise to simultaneously achieve high efficiency and long-term operation in IPV's application. However, the dearth of polymer acceptors with medium-bandgap has impeded the rapid development of indoor all-PSCs. Herein, a highly efficient medium-bandgap polymer acceptor (PYFO-V) is reported through the synergistic effects of side chain engineering and linkage modulation and applied for indoor all-PSCs operation. As a result, the PM6:PYFO-V-based indoor all-PSC yields the highest efficiency of 27.1% under LED light condition, marking the highest value for reported binary indoor all-PSCs to date. More importantly, the blade-coated devices using non-halogenated solvent (o-xylene) maintain an efficiency of over 23%, demonstrating the potential for industry-scale fabrication. This work not only highlights the importance of fine-tuning intramolecular charge transfer effect and intrachain coplanarity in developing high-performance medium-bandgap polymer acceptors but also provides a highly efficient strategy for indoor all-PSC application., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Power conversion efficiency (PCE) of organic solar cells (OSCs) processed by nonhalogenated solvents is unsatisfactory due to the unfavorable morphology. Herein, two new small molecule acceptors (SMAs) Y6-Ph and L8-Ph are synthesized by introducing a phenyl end group in the inner side chains of the SMAs of Y6 and L8-BO, respectively, for overcoming the excessive aggregation of SMAs in the long-time film forming processed by nonhalogenated solvents. First, the effect of the film forming time on the aggregation property and photovoltaic performance of Y6, L8-BO, Y6-Ph, and L8-Ph is studied by using the commonly used solvents: chloroform (CF) (rapid film forming process) and chlorobenzene (CB) (slow film forming process). It is found that Y6- and L8-BO-based OSCs exhibit a dramatic drop in PCE from CF- to CB-processed devices owing to the large phase separation, while the Y6-Ph and L8-Ph based OSCs show obviously increased PCEs Furthermore, L8-Ph-based OSCs processed by nonhalogenated solvent o-xylene (o-XY) achieved a high PCE of 18.40% with an FF of 80.11%. The results indicate that introducing a phenyl end group in the inner side chains is an effective strategy to modulate the morphology and improve the photovoltaic performance of the OSCs processed by nonhalogenated solvents., (© 2023 Wiley-VCH GmbH.)

Mixing a sterically bulky, electron-transporting host material into a conventional single host-guest emissive layer is demonstrated to suppress phase separation of the host matrix while increasing the efficiency and operational lifetime of deep-blue phosphorescent organic light-emitting diodes (PHOLEDs) with chromaticity coordinates of (0.14, 0.15). The bulky host enables homogenous mixing of the molecules comprising the emissive layer while suppressing single host aggregation; a significant loss channel of nonradiative recombination. By controlling the amorphous phase of the host-matrix morphology, the mixed-host device achieves a significant reduction in nonradiative exciton decay, resulting in 120 ± 6% increase in external quantum efficiency relative to an analogous, single-host device. In contrast to single host PHOLEDs where electrons are transported by the host and holes by the dopants, both charge carriers are conducted by the mixed host, reducing the probability of exciton annihilation, thereby doubling of the deep-blue PHOLED operational lifetime. These findings demonstrate that the host matrix morphology affects almost every aspect of PHOLED performance., (© 2023 Wiley-VCH GmbH.)

A major challenge hindering the further development of all-polymer solar cells (all-PSCs) employing polymerized small-molecule acceptors is the relatively low fill factor (FF) due to the difficulty in controlling the active-layer morphology. The issues typically arise from oversized phase separation resulting from the thermodynamically unfavorable mixing between two macromolecular species, and disordered molecular orientation/packing of highly anisotropic polymer chains. Herein, a facile top-down controlling strategy to engineer the morphology of all-polymer blends is developed by leveraging the layer-by-layer (LBL) deposition. Optimal intermixing of polymer components can be achieved in the two-step process by tuning the bottom-layer polymer swelling during top-layer deposition. Consequently, both the molecular orientation/packing of the bottom layer and the molecular ordering of the top layer can be optimized with a suitable top-layer processing solvent. A favorable morphology with gradient vertical composition distribution for efficient charge transport and extraction is therefore realized, affording a high all-PSC efficiency of 17.0% with a FF of 76.1%. The derived devices also possess excellent long-term thermal stability and can retain >90% of their initial efficiencies after being annealed at 65 °C for 1300 h. These results validate the distinct advantages of employing an LBL processing protocol to fabricate high-performance all-PSCs., (© 2022 Wiley-VCH GmbH.)

A record power conversion efficiency (PCE) of over 19% is realized in planar-mixed heterojunction (PMHJ) organic solar cells (OSCs) by adopting the asymmetric selenium substitution strategy in making a pseudosymmetric electron acceptor, BS3TSe-4F. The combined molecular asymmetry with more polarizable selenium substitution increases the dielectric constant of the D18/BS3TSe-4F blend, helping lower the exciton binding energy. On the other hand, dimer packing in BS3TSe-4F is facilitated to enable free charge generation, helping more efficient exciton dissociation and lowering the radiative recombination loss (ΔE 2 ) of OSCs. As a result, PMHJ OSCs based on D18/BS3TSe-4F achieve a PCE of 18.48%. By incorporating another mid-bandgap acceptor Y6-O into D18/BS3TSe-4F to form a ternary PMHJ, a higher open-circuit voltage (V OC ) can be achieved to realize an impressive PCE of 19.03%. The findings of using pseudosymmetric electron acceptors in enhancing device efficiency provides an effective way to develop highly efficient acceptor materials for OSCs., (© 2022 Wiley-VCH GmbH.)

All-polymer solar cells (all-PSCs) have drawn growing attention and achieved tremendous progress recently, but their power conversion efficiency (PCE) still lags behind small-molecule-acceptor (SMA)-based PSCs due to the relative difficulty on morphology control of polymer photoactive blends. Here, low-cost PTQ10 is introduced as a second polymer donor (a third component) into the PM6:PY-IT blend to finely tune the energy-level matching and microscopic morphology of the polymer blend photoactive layer. The addition of PTQ10 decreases the π-π stacking distance, and increases the π-π stacking coherence length and the ordered face-on molecular packing orientation, which improves the charge separation and transport in the photoactive layer. Moreover, the deeper highest occupied molecular orbital energy level of the PTQ10 polymer donor than PM6 leads to higher open-circuit voltage of the ternary all-PSCs. As a result, a PCE of 16.52% is achieved for ternary all-PSCs, which is one of the highest PCEs for all-PSCs. In addition, the ternary devices exhibit a high tolerance of the photoactive layer thickness with high PCEs of 15.27% and 13.91% at photoactive layer thickness of ≈205 and ≈306 nm, respectively, which are the highest PCEs so far for all-PSCs with a thick photoactive layer., (© 2022 Wiley-VCH GmbH.)

In all-small-molecule organic solar cells (ASM-OSCs), a high short-circuit current (J sc ) usually needs a small phase separation, while a high fill factor (FF) is generally realized in a highly ordered packing system. However, small domain and ordered packing always conflicted each other in ASM-OSCs, leading to a mutually restricted J sc and FF. In this study, alleviation of the previous dilemma by the strategy of obtaining simultaneous good miscibility and ordered packing through modulating homo- and heteromolecular interactions is proposed. By moving the alkyl-thiolation side chains from the para- to the meta-position in the small-molecule donor, the surface tension and molecular planarity are synchronously enhanced, resulting in compatible properties of good miscibility with acceptor BTP-eC9 and strong self-assembly ability. As a result, an optimized morphology with multi-length-scale domains and highly ordered packing is realized. The device exhibits a long carrier lifetime (39.8 μs) and fast charge collection (15.5 ns). A record efficiency of 16.2% with a high FF of 75.6% and a J sc of 25.4 mA cm -2 in the ASM-OSCs is obtained. These results demonstrate that the strategy of simultaneously obtaining good miscibility with high crystallinity could be an efficient photovoltaic material design principle for high-performance ASM-OSCs., (© 2021 Wiley-VCH GmbH.)

Solution-processed organic semiconductor charge-transport layers (OS-CTLs) with high mobility, low trap density, and energy level alignment have dominated the important progress in p-i-n planar perovskite solar cells (pero-SCs). Unfortunately, their inevitable long chains result in weak molecular stacking, which is likely to generate high energy disorder and deteriorate the charge-transport ability of OS-CTLs. Here, a charge-transfer complex (CTC) strategy to reduce the energy disorder in the OS-CTLs by doping an organic semiconductor, 4,4'-(4,8-bis(5-(trimethylsilyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)bis(N,N-bis(4-methoxyphenyl)aniline) (BDT-Si), in a commercial hole-transport layer (HTL), poly[bis(4-phenyl) (2,4,6-trimethylphenyl)amine (PTAA), is proposed. The formation of the CTC makes the PTAA conjugated backbone electron-deficient, resulting in a quinoidal and stiffer character, which is likely to planarize the PTAA backbone and enhance the ordering of the film in nanoscale. The resultant HTL exhibits a reduced energy disorder, which simultaneously promotes hole transport in the HTL, hole extraction at the interface, energy level alignment, and quasi-Fermi level splitting in the device. As a result, the p-i-n planar pero-SCs with optimized HTL exhibit the best power conversion efficiency of 21.87% with good operating stability. This finding demonstrates that the CTC strategy is an effective way to reduce the energy disorder in HTLs and to improve the performance of planar pero-SCs., (© 2021 Wiley-VCH GmbH.)

Developing high-performance donor polymers is important for nonfullerene organic solar cells (NF-OSCs), as state-of-the-art nonfullerene acceptors can only perform well if they are coupled with a matching donor with suitable energy levels. However, there are very limited choices of donor polymers for NF-OSCs, and the most commonly used ones are polymers named PM6 and PM7, which suffer from several problems. First, the performance of these polymers (particularly PM7) relies on precise control of their molecular weights. Also, their optimal morphology is extremely sensitive to any structural modification. In this work, a family of donor polymers is developed based on a random polymerization strategy. These polymers can achieve well-controlled morphology and high-performance with a variety of chemical structures and molecular weights. The polymer donors are D-A1-D-A2-type random copolymers in which the D and A1 units are monomers originating from PM6 or PM7, while the A2 unit comprises an electron-deficient core flanked by two thiophene rings with branched alkyl chains. Consequently, multiple cases of highly efficient NF-OSCs are achieved with efficiencies between 16.0% and 17.1%. As the electron-deficient cores can be changed to many other structural units, the strategy can easily expand the choices of high-performance donor polymers for NF-OSCs., (© 2020 Wiley-VCH GmbH.)

With power conversion efficiency now over 17%, a long operational lifetime is essential for the successful application of organic solar cells. However, most non-fullerene acceptors can crystallize and destroy devices, yet the fundamental underlying thermodynamic and kinetic aspects of acceptor crystallization have received limited attention. Here, room-temperature (RT) diffusion coefficients of 3.4 × 10 -23 and 2.0 × 10 -22 are measured for ITIC-2Cl and ITIC-2F, two state-of-the-art non-fullerene acceptors. The low coefficients are enough to provide for kinetic stabilization of the morphology against demixing at RT. Additionally profound differences in crystallization characteristics are discovered between ITIC-2F and ITIC-2Cl. The differences as observed by secondary-ion mass spectrometry, differential scanning calorimetry (DSC), grazing-incidence wide-angle X-ray scattering, and microscopy can be related directly to device degradation and are attributed to the significantly different nucleation and growth rates, with a difference in the growth rate of a factor of 12 at RT. ITIC-4F and ITIC-4Cl exhibit similar characteristics. The results reveal the importance of diffusion coefficients and melting enthalpies in controlling the growth rates, and that differences in halogenation can drastically change crystallization kinetics and device stability. It is furthermore delineated how low nucleation density and large growth rates can be inferred from DSC and microscopy experiments which could be used to guide molecular design for stability., (© 2020 Wiley-VCH GmbH.)

Organic solar cells (OSCs) based on D18:Y6 have recently exhibited a record power conversion efficiency of over 18%. The initial work is extended and the device performance of D18-based OSCs is compared with three non-fullerene acceptors, Y6, IT-4F, and IEICO-4Cl, and their molecular packing characteristics and miscibility are studied. The D18 polymer shows unusually strong chain extension and excellent backbone ordering in all films, which likely contributes to the excellent hole-transporting properties. Thermodynamic characterization indicates a room-temperature miscibility for D18:Y6 and D18:IT-4F near the percolation threshold. This corresponds to an ideal quench depth and explains the use of solvent vapor annealing rather than thermal annealing. In contrast, D18:IEICO-4Cl is a low-miscibility system with a deep quench depth during casting and poor morphology control and low performance. A failure of ternary blends with PC 71 BM is likely due to the near-ideal miscibility of Y6 to begin with and indicates that strategies for developing successful ternary or quaternary solar cells are likely very different for D18 than for other high-performing donors. This work reveals several unique property-performance relations of D18-based photovoltaic devices and helps guide design or fabrication of yet higher efficiency OSCs., (© 2020 Wiley-VCH GmbH.)

Quasi-2D Ruddlesden-Popper halide perovskites with a large exciton binding energy, self-assembled quantum wells, and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi-2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower-dimensional nanosheets (high-bandgap domains) to 3D nanocrystals (low-bandgap domains). High-quality quasi-2D perovskite (PEA) 2 (FA) 3 Pb 4 Br 13 films are fabricated by solution engineering. Grazing-incidence wide-angle X-ray scattering measurements are conducted to study the crystal orientation, and transient absorption spectroscopy measurements are conducted to study the charge-carrier dynamics. These data show that highly oriented 2D crystal films have a faster energy transfer from the high-bandgap domains to the low-bandgap domains (<0.5 ps) compared to the randomly oriented films. High-performance light-emitting diodes can be realized with these highly oriented 2D films. Finally, amplified spontaneous emission with a low threshold 4.16 µJ cm -2 is achieved and distributed feedback lasers are also demonstrated. These results show that it is important to control the morphology of the quasi-2D films to achieve efficient energy transfer, which is a critical requirement for light-emitting devices., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Casting of a donor:acceptor bulk-heterojunction structure from a single ink has been the predominant fabrication method of organic photovoltaics (OPVs). Despite the success of such bulk heterojunctions, the task ofcontrolling the microstructure in a single casting process has been arduous and alternative approaches are desired. To achieve OPVs with a desirable microstructure, a facile and eco-compatible sequential deposition approach is demonstrated for polymer/small-molecule pairs. Using a nominally amorphous polymer as the model material, the profound influence of casting solvent is shown on the molecular ordering of the film, and thus the device performance and mesoscale morphology of sequentially deposited OPVs can be tuned. Static and in situ X-ray scattering indicate that applying (R)-(+)-limonene is able to greatly promote the molecular order of weakly crystalline polymers and form the largest domain spacing exclusively, which correlates well with the best efficiency of 12.5% in sequentially deposited devices. The sequentially cast device generally outperforms its control device based on traditional single-ink bulk-heterojunction structure. More crucially, a simple polymer:solvent interaction parameter χ is positively correlated with domain spacing in these sequentially deposited devices. These findings shed light on innovative approaches to rationally create environmentally friendly and highly efficient electronics., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Organic solar cells (OSCs) are one of the most promising cost-effective options for utilizing solar energy, and, while the field of OSCs has progressed rapidly in device performance in the past few years, the stability of nonfullerene OSCs has received less attention. Developing devices with both high performance and long-term stability remains challenging, particularly if the material choice is restricted by roll-to-roll and benign solvent processing requirements and desirable mechanical durability. Building upon the ink (toluene:FTAZ:IT-M) that broke the 10% benchmark when blade-coated in air, a second donor material (PBDB-T) is introduced to stabilize and enhance performance with power conversion efficiency over 13% while keeping toluene as the solvent. More importantly, the ternary OSCs exhibit excellent thermal stability and storage stability while retaining high ductility. The excellent performance and stability are mainly attributed to the inhibition of the crystallization of nonfullerene small-molecular acceptors (SMAs) by introducing a stiff donor that also shows low miscibility with the nonfullerene SMA and a slightly higher highest occupied molecular orbital (HOMO) than the host polymer. The study indicates that improved stability and performance can be achieved in a synergistic way without significant embrittlement, which will accelerate the future development and application of nonfullerene OSCs., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Two medium-bandgap p-type organic small molecules H21 and H22 with an alkylsily-thienyl conjugated side chain on benzo[1,2-b:4,5-b']dithiophene central units are synthesized and used as donors in all-small-molecule organic solar cells (SM-OSCs) with a narrow-bandgap n-type small molecule 2,2'-((2Z,2'Z)-((4,4,9,9-tetrahexyl-4,9-dihydro-s-indaceno[1,2-b:5,6-b']dithiophene-2,7-diyl)bis(methanylylidene))bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (IDIC) as the acceptor. In comparison to H21 with 3-ethyl rhodanine as the terminal group, H22 with cyanoacetic acid esters as the terminal group shows blueshifted absorption, higher charge-carrier mobility and better 3D charge pathway in blend films. The power conversion efficiency (PCE) of the SM-OSCs based on H22:IDIC reaches 10.29% with a higher open-circuit voltage of 0.942 V and a higher fill factor of 71.15%. The PCE of 10.29% is among the top efficiencies of nonfullerene SM-OSCs reported in the literature to date., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Besides broadening of the absorption spectrum, modulating molecular energy levels, and other well-studied properties, a stronger intramolecular electron push-pull effect also affords other advantages in nonfullerene acceptors. A strong push-pull effect improves the dipole moment of the wings in IT-4F over IT-M and results in a lower miscibility than IT-M when blended with PBDB-TF. This feature leads to higher domain purity in the PBDB-TF:IT-4F blend and makes a contribution to the better photovoltaic performance. Moreover, the strong push-pull effect also decreases the vibrational relaxation, which makes IT-4F more promising than IT-M in reducing the energetic loss of organic solar cells. Above all, a power conversion efficiency of 13.7% is recorded in PBDB-TF:IT-4F-based devices., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The commercialization of nonfullerene organic solar cells (OSCs) critically relies on the response under typical operating conditions (for instance, temperature and humidity) and the ability of scale-up. Despite the rapid increase in power conversion efficiency (PCE) of spin-coated devices fabricated in a protective atmosphere, the efficiencies of printed nonfullerene OSC devices by blade coating are still lower than 6%. This slow progress significantly limits the practical printing of high-performance nonfullerene OSCs. Here, a new and relatively stable nonfullerene combination is introduced by pairing the nonfluorinated acceptor IT-M with the polymeric donor FTAZ. Over 12% efficiency can be achieved in spin-coated FTAZ:IT-M devices using a single halogen-free solvent. More importantly, chlorine-free, blade coating of FTAZ:IT-M in air is able to yield a PCE of nearly 11% despite a humidity of ≈50%. X-ray scattering results reveal that large π-π coherence length, high degree of face-on orientation with respect to the substrate, and small domain spacing of ≈20 nm are closely correlated with such high device performance. The material system and approach yield the highest reported performance for nonfullerene OSC devices by a coating technique approximating scalable fabrication methods and hold great promise for the development of low-cost, low-toxicity, and high-efficiency OSCs by high-throughput production., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Improving the fill factor (FF) is known as a challenging issue in organic solar cells (OSCs). Herein, a strategy of extending the conjugated area of end-group is proposed for the molecular design of acceptor-donor-acceptor (A-D-A)-type small molecule acceptor (SMA), and an indaceno[1,2-b:5,6-b']dithiophene-based SMA, namely IDTN, by end-capping with the naphthyl fused 2-(3-oxocyclopentylidene)malononitrile is synthesized. Benefiting from the π-conjugation extension by fusing two phenyls, IDTN shows stronger molecular aggregation, more ordered packing structure, thus over one order of magnitude higher electron mobility relative to its counterpart. By utilizing the fluorinated polymer (PBDB-TF) as the electron donor, the corresponding device exhibits a high efficiency of 12.2% with a record-high FF of 0.78, which is approaching the theoretical limit of OSCs. Compared with the reference molecule, such a high FF in the IDTN system can be mainly attributed to the more ordered π-π packing of acceptor aggregates, higher domain purity and symmetric carrier transport in the blend. Hence, enlarging the conjugated area of the terminal-group in these A-D-A-type SMAs is a promising approach not only for enhancing the electron mobility, but also for improving the blend morphology, and both of them are conducive to the fill-factor breakthrough., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A new polymer acceptor, naphthodiperylenetetraimide-vinylene (NDP-V), featuring a backbone of altenating naphthodiperylenetetraimide and vinylene units is designed and applied in all-polymer solar cells (all-PSCs). With this polymer acceptor, a new record power-conversion efficiencies (PCE) of 8.59% has been achieved for all-PSCs. The design principle of NDP-V is to reduce the conformational disorder in the backbone of a previously developed high-performance acceptor, PDI-V, a perylenediimide-vinylene polymer. The chemical modifications result in favorable changes to the molecular packing behaviors of the acceptor and improved morphology of the donor-acceptor (PTB7-Th:NDP-V) blend, which is evidenced by the enhanced hole and electron transport abilities of the active layer. Moreover, the stronger absorption of NDP-V in the shorter-wavelength range offers a better complement to the donor. All these factors contribute to a short-circuit current density (J sc ) of 17.07 mA cm -2 . With a fill factor (FF) of 0.67, an average PCE of 8.48% is obtained, representing the highest value thus far reported for all-PSCs., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A new acceptor-donor-acceptor-structured nonfullerene acceptor ITCC (3,9-bis(4-(1,1-dicyanomethylene)-3-methylene-2-oxo-cyclopenta[b]thiophen)-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d':2,3-d']-s-indaceno[1,2-b:5,6-b']-dithiophene) is designed and synthesized via simple end-group modification. ITCC shows improved electron-transport properties and a high-lying lowest unoccupied molecular orbital level. A power conversion efficiency of 11.4% with an impressive V OC of over 1 V is recorded in photovoltaic devices, suggesting that ITCC has great potential for applications in tandem organic solar cells., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A wide bandgap small molecular acceptor, SFBRCN, containing a 3D spirobifluorene core flaked with a 2,1,3-benzothiadiazole (BT) and end-capped with highly electron-deficient (3-ethylhexyl-4-oxothiazolidine-2-yl)dimalononitrile (RCN) units, has been successfully synthesized as a small molecular acceptor (SMA) for nonfullerene polymer solar cells (PSCs). This SMA exhibits a relatively wide optical bandgap of 2.03 eV, which provides a complementary absorption to commonly used low bandgap donor polymers, such as PTB7-Th. The strong electron-deficient BT and RCN units afford SFBRCN with a low-lying LUMO (lowest unoccupied molecular orbital) level, while the 3D structured spirobifluorene core can effectively suppress the self-aggregation tendency of the SMA, thus yielding a polymer:SMA blend with reasonably small domain size. As the results of such molecular design, SFBRCN enables nonfullerene PSCs with a high efficiency of 10.26%, which is the highest performance reported to date for a large bandgap nonfullerene SMA., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Fullerene-free organic solar cells show over 11% power conversion efficiency, processed by low toxic solvents. The applied donor and acceptor in the bulk heterojunction exhibit almost the same highest occupied molecular orbital level, yet exhibit very efficient charge creation., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A sequential-casting ternary method is developed to create stratified bulk heterojunction (BHJ) solar cells, in which the two BHJ layers are spin cast sequentially without the need of adopting a middle electrode and orthogonal solvents. This method is found to be particularly useful for polymers that form a mechanically alloyed morphology due to the high degree of miscibility in the blend., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Fine energy-level modulations of small-molecule acceptors (SMAs) are realized via subtle chemical modifications on strong electron-withdrawing end-groups. The two new SMAs (IT-M and IT-DM) end-capped by methyl-modified dicycanovinylindan-1-one exhibit upshifted lowest unoccupied molecular orbital (LUMO) levels, and hence higher open-circuit voltages can be observed in the corresponding devices. Finally, a top power conversion efficiency of 12.05% is achieved., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

All-polymer solar cells with 7.57% power conversion efficiency are achieved via a new perylenediimide-based polymeric acceptor. Furthermore, the device processed in ambient air without encapsulation can still reach a high power conversion efficiency (PCE) of 7.49%, which is a significant economic advantage from an industrial processing perspective. These results represent the highest PCE achieved from perylenediimide-based polymers., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A difluorobenzoxadiazole building block is synthesized and utilized to construct a conjugated polymer leading to high-performance thick-film polymer solar cells with a V(OC) of 0.88 V and a power conversion efficiency of 9.4%. This new building block can be used in many possible polymer structures for various organic electro-nic applications., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A novel, yet simple solution fabrication technique to address the trade-off between photocurrent and fill factor in thick bulk heterojunction organic solar cells is described. The inverted off-center spinning technique promotes a vertical gradient of the donor-acceptor phase-separated morphology, enabling devices with near 100% internal quantum efficiency and a high power conversion efficiency of 10.95%., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Rigid fused perylene diimide (PDI) dimers bridged with heterocycles exhibit superior photovoltaic performance compared to their unfused semiflexible analogues. Changing the chalcogen atoms in the aromatic bridges gradually increases the twist angles between the two PDI planes, leading to a varied morphology in which the one bridged by thiophene achieves a balance and shows the best efficiency of 6.72%., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A 7.3% efficiency non-fullerene polymer solar cell is realized by combining a large-bandgap polymer PffT2-FTAZ-2DT with a small-bandgap acceptor IEIC. The complementary absorption of donor polymer and small-molecule acceptor is responsible for the high-performance of the solar-cell device. This work provides important guidance to improve the performance of non-fullerene polymer solar cells., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Manipulating molecular orientation at the donor/acceptor interface is the key to boosting charge separation properties and efficiencies of anisotropic-materials-based organic photovoltaics (OPVs). By replacing the polymeric donor PBDTBDD with its 2D-conjugated polymer PBDTBDD-T, the power conversion efficiency of OPVs featuring the anisotropic polymer acceptor PNDI is drastically boosted from 2.4% up to 5.8%., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A new copolymer PM6 based on fluorothienyl-substituted benzodithiophene is synthesized and characterized. The inverted polymer solar cells based on PM6 exhibit excellent performance with Voc of 0.98 V and power conversion efficiency (PCE) of 9.2% for a thin-film thickness of 75 nm. Furthermore, the single-junction semitransparent device shows a high PCE of 5.7%., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Connections are delineated between solar-cell performance, charge-carrier mobilities, and morphology in a highperformance molecular solar cell. The observations show that maximizing the relative phase purity and structural order while simultaneously limiting the domain size may be essential for achieving optimal solar-cell performances in solution-processed small-molecule solar cells ., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A relationship between solvent additive concentration and active layer thickness in small-molecule solar cells is investigated. Specifically, the additive concentration must scale with the amount of semiconductor material and not as absolute concentration in solution. Devices with a wide range of active layers with thickness up to 200 nm can readily achieve efficiencies close to 6% when the right concentration of additive is used., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

All-polymer solar cells based on a pair of crystalline low-bandgap polymers (NT and N2200) are demonstrated to achieve a high short-circuit current density of 11.5 mA cm-2 and a power conversion efficiency of up to 5.0% under the standard AM1.5G spectrum with one sun intensity. The high performance of these NT:N2200-based cells can be attributed to the low optical bandgaps of the polymers and the reasonably high and balanced electron and hole mobilities of the NT:N2200 blends due to the crystalline nature of the two polymers., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A polythiophene derivative called PDCBT, which has a backbone of thiophene units and just carboxylate functional groups to modulate its properties, exhibits properties superior to those of poly(3-hexylthiophene), the classic polythiophene derivative, when used as an electron donor in polymer solar cells (PSCs). The best device, based on PDCBT/PC71BM (1:1), develops a good power conversion efficiency of 7.2%., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The molecular weight (MW) of PBnDT-FTAZ can be precisely controlled by adjusting the stoichiometric ratio of the two monomers, following the Carothers equation. The study of a set of PBnDT-FTAZ polymers with different MWs reveals that the MW significantly influences the morphology and structural order of PBnDTFTAZ in its bulk heterojunction solar cells, with the highest efficiency (over 7%) achieved with the use of a MW of 40 000 g mol(-1) ., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The addition of small quantities of polystyrene (PS) is a simple and economically viable process that improves the power conversion efficiency of one of the most efficient small molecule donors. Addition of PS increases the solution viscosity, thereby providing thicker layers, and allows the formation of a desirable bulk heterojunction morphology. Moreover, the PS spontaneously accumulates as phase separated domains, away from the electrodes, so as not to interfere with charge extraction., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

For the blend film of PBDTTT-C-T:PC71 BM, the use of 1,8-diiodooctane as the solvent additive enriches the polymer at the top surface, so that a power conversion efficiency of 9.13% is recorded in the inverted polymer solar cell based on the blend, which is much higher than that of the device with conventional structure., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The field dependence and yield of free charge carrier generation in polymer:fullerene blends with varying energetic offsets is not affected when the excitation energy is varied from above band-gap to direct CT state excitation. Instead, the ability of the CT state to split is dictated by the energetic offset between the relaxed CT state and the charge separated (CS) state., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Attaching meta-alkoxy-phenyl groups as conjugated side chains is an easy and effective way to modulate the molecular energy level of D-A polymer for photovoltaic application, and the polymer solar cells based on the polymer consisting meta-alkoxy-phenyl groups as conjugated side chain, PBT-OP, shows an enhanced open circuit voltage and thus higher efficiency of 7.50%, under the illumination of AM 1.5G, 100 mW/cm(2) ., (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The correlation among molecular conformation, the crystallinity of the morphology, propensity for π-π stacking, J- versus H-aggregation, and photovoltaic performance have been studied based on two newly designed polymers, PBDTTT-S-T and PDT-S-T. The results show that more linear backbone structure is helpful to improve photovoltaic properties of the polymer, and therefore, molecular conformation should be considered for molecular design of photovoltaic polymers., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

For the PDPP3T/PCBM system investigated here, atomic force microscopy, resonant soft X-ray scattering, and grazing incidence wide angle X-ray scattering are used as an initial set of tools to determine the surface texture, the bulk compositional morphology, and the crystallization behavior, respectively. We find systematic variations and relate them to device performance. A solvent mixture of DCB/CF/DIO = 76:19:5 (v/v/v) yields a PCE of 6.71%., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)