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Two-dimensional (2D) organic−inorganic hybrid perovskites (OIHPs) have showed impressive stability, compared to their three-dimensional (3D) counterparts. However, tuning the chemical structure of the organic cations to simultaneously improve the device performance and stability of 2D OIHP solar cells is rarely reported. Here, we demonstrate that by introducing a classic noncovalent aryl-perfluoroaryl interaction, 2D OIHP solar cells with 1:1 mixed phenethylammonium (PEA) and perfluorophenethylammonium (F5-PEA) can achieve an efficiency of >10% with much enhanced stability using a simple deposition at low temperature without using any additives. The competing effects of surface morphology and crystal orientation with an increased amount of F5-PEA result in the highest efficiency at a 1:1 ratio, while single-crystal studies reveal the expected aryl-perfluoroaryl interaction, accounting for the highest device stability of 2D OIHP solar cell at 1:1 ratio as well. This work provides an example where tuning the interactions of organic cations via molecular engineering can have a profound effect on device performance and stability of 2D OIHP solar cells.

Summary Herein, we report ternary organic solar cells with a power conversion efficiency (PCE) of 14.0%. By incorporating 10 wt % of BIT-4F-T in the PTB7-Th:IEICO-4F blend, we obtain an enhancement of all photovoltaic parameters compared to the binary devices, leading to a 15% performance improvement in ternary blend. The high photocurrent in 10% BIT-4F-T blend results from a complementary absorption profile of donor components and a hole transfer from BIT-4F-T to PTB7-Th. Morphological and device characterizations reveal that the addition of 10% BIT-4F-T acts not only as a sensitizer but also as a solid processing aid, which is beneficial for charge generation and transport. The effect of the third component is observed in different non-fullerene and fullerene OSCs. Our study demonstrates that careful selection of a third component, where dual sensitizing and processing-aid effects are observed, can be a design strategy to achieve a concomitant improvement in all photovoltaic parameters.

The short exciton diffusion length associated with most classical organic semiconductors used in organic photovoltaics (5-20 nm) imposes severe limits on the maximum size of the donor and acceptor domains within the photoactive layer of the cell. Identifying materials that are able to transport excitons over longer distances can help advancing our understanding and lead to solar cells with higher efficiency. Here, we measure the exciton diffusion length in a wide range of nonfullerene acceptor molecules using two different experimental techniques based on photocurrent and ultrafast spectroscopy measurements. The acceptors exhibit balanced ambipolar charge transport and surprisingly long exciton diffusion lengths in the range of 20 to 47 nm. With the aid of quantum-chemical calculations, we are able to rationalize the exciton dynamics and draw basic chemical design rules, particularly on the importance of the end-group substituent on the crystal packing of nonfullerene acceptors., The short-range diffusion length of organic semiconductors severely limits exciton harvesting and charge generation in organic bulk heterojunction solar cells. Here, the authors report exciton diffusion length in the range of 20 to 47 nm for a wide range of non-fullerene acceptors molecules.

Solution-processed Cu(In,Ga)(S,Se)

High-performance low-band-gap polymer semiconductors are visibly colored, making them unsuitable for transparent and imperceptible electronics without reducing film thickness to the nanoscale range. Herein, we demonstrate polymer/insulator blends exhibiting favorable miscibility that improves the transparency and carrier transport in an organic field-effect transistor (OFET) device. The mesoscale structures leading to more efficient charge transport in ultrathin films relevant to the realization of transparent and flexible electronic applications are explored based on thermodynamic material interaction principles in conjunction with optical and morphological studies. By blending the commodity polymer polystyrene (PS) with two high-performing polymers, PDPP3T and P (NDI2OD-T2) (known as N2200), a drastic difference in morphology and fiber network are observed due to considerable differences in the degree of thermodynamic interaction between the conjugated polymers and PS. Intrinsic material interaction behavior establishes a long-range intermolecular interaction in the PDPP3T polymer fibrillar network dispersed in the majority (80%) PS matrix resulting in a ca. 3-fold increased transistor hole mobility of 1.15 cm2 V-1 s-1 (highest = 1.5 cm2 V-1 s-1) as compared to the pristine material, while PS barely affects the electron mobility in N2200. These basic findings provide important guidelines to achieve high mobility in transparent OFETs.

Layered perovskites have been shown to improve the stability of perovskite solar cells while its operation mechanism remains unclear. Here we investigate the process for the conversion of light to electrical current in high performance layered perovskite solar cells by examining its real morphology. The layered perovskite films in this study are found to be a mixture of layered and three dimensional (3D)-like phases with phase separations at micrometer and nanometer scale in both vertical and lateral directions. This phase separation is explained by the surface initiated crystallization process and the competition of the crystallization between 3D-like and layered perovskites. We further propose that the working mechanisms of the layered perovskite solar cells involve energy transfer from layered to 3D-like perovskite network. The impact of morphology on efficiency and stability of the hot-cast layered perovskite solar cells are also discussed to provide guidelines for the future improvement., It is well-accepted that the two dimensional layered halide perovskite can improve the device stability of perovskite solar cells but the operation mechanism remains unclear. Here Lin et al. reveal the real morphology of the hot-cast layered perovskite solar cells and understand the working mechanism.

Two-dimensional perovskites have emerged as more intrinsically stable materials for solar cells. Chemical tuning of spacer organic cations has attracted great interest due to their additional functionalities. However, how the chemical nature of the organic cations affects the properties of two-dimensional perovskites and devices is rarely reported. Here we demonstrate that the selection of spacer cations (i.e., selective fluorination of phenethylammonium) affects the film properties of two-dimensional perovskites, leading to different device performance of two-dimensional perovskite solar cells (average n = 4). Structural analysis reveals that different packing arrangements and orientational disorder of the spacer cations result in orientational degeneracy and different formation energies, largely explaining the difference in film properties. This work provides key missing information on how spacer cations exert influence on desirable electronic properties and device performance of two-dimensional perovskites via the weak and cooperative interactions of these cations in the crystal lattice., Two dimensional halide perovskites solar cells have attracted research interest due to their higher stability compared to three dimensional counterparts. Here Hu et al. show that fine tuning of the chemical structure of the spacer cations leads to different packing arrangements and device efficiency.

We demonstrate a new method to reverse the polarity and charge transport behavior of naphthalenediimide (NDI)-based copolymers by inserting a vinylene linker between the donor and acceptor units. The vinylene linkers minimize the intrinsic steric congestion between the NDI and thiophene moieties to prompt backbone planarity. The polymers with vinylene linkers exhibit electron n-channel transport characteristics under vacuum, similar to the benchmark polymer, P(NDI2OD-T2). To our surprise, when the polymers are measured in air, the dominant carrier type switches from n- to p-type and yield hole mobilities up to 0.45 cm2 V–1 s–1 with hole to electron mobility ratio of three (μh/μe, ∼3), which indicates that the hole density in the active layer can be significantly increased by exposure to air. This increase is consistent with the intrinsic more delocalized nature of the highest occupied molecular orbital of the charged vinylene polymer, as estimated by density functional theory (DFT) calculations, which fac...

This feature article provides a general introduction to Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy of conjugated polymers as well as a perspective on the information that NEXAFS spectroscopy is able to provide. While conjugated polymers are of interest for a range of applications including organic light-emitting diodes, polymer solar cells and organic field-effect transistors (OFETs), this feature article will focus on the application of NEXAFS spectroscopy for revealing information about the interfacial orientation and alignment of conjugated polymer chains with respect to substrate surfaces which is of particular relevance for understanding charge transport through the thin accumulation layer in a polymer OFET. The potential for NEXAFS spectroscopy to provide experimental information about dihedral angles in donor–acceptor copolymers is also highlighted.

An ambipolar poly(diketopyrrolopyrrole-terthiophene)-based field-effect transistor (FET) sensitively detects xylene isomers at low ppm levels with multiple sensing features. Combined with pattern-recognition algorithms, a sole ambipolar FET sensor, rather than arrays of sensors, can discriminate highly similar xylene structural isomers from one another.

Solution-processed Cu(In,Ga)(S,Se)2 (CIGS) has a great potential for the production of large-area photovoltaic devices at low cost. However, CIGS solar cells processed from solution exhibit relatively lower performance compared to vacuum-processed devices because of a lack of proper composition distribution, which is mainly instigated by the limited Se uptake during chalcogenization. In this work, a unique potassium treatment method is utilized to improve the selenium uptake judiciously, enhancing grain sizes and forming a wider bandgap minimum region. Careful engineering of the bandgap grading structure also results in an enlarged space charge region, which is favorable for electron-hole separation and efficient charge carrier collection. Besides, this device processing approach has led to a linearly increasing electron diffusion length and carrier lifetime with increasing the grain size of the CIGS film, which is a critical achievement for enhancing photocurrent yield. Overall, 15% of power conversion efficiency is achieved in solar cells processed from environmentally benign solutions. This approach offers critical insights for precise device design and processing rules for solution-processed CIGS solar cells.

Organically modified chalcogenide (ORMOCHALC) polymers have proven to be alternatives to the conventional inorganic materials for mid-wavelength infrared (MWIR, λ = 3–5 μm) optical components. While the refractive index of ORMOCHALC can be reinforced by the content of chalcogenides such as sulfur (S) and selenium (Se), the increased portion of the S or Se deteriorate the thermomechanical stabilities. As a remedy, this study utilizes ZnS nanoparticles to reinforce both optical and thermomechanical properties of the sulfur-based ORMOCHALC polymer, poly(S-random-1,3-diisopropenylbenzene). The refractive index n and extinction coefficient k of the nanocomposites were characterized by Infrared Variable Angle Spectroscopic Ellipsometry (IR-VASE). The results show a significant increment in the refractive index of Δn = 6.58% at the wavelength of 4 μm by adding 20 wt% ZnS (or 7.29 vol%) in the ORMOCHALC polymer. The low extinction coefficient of the nanocomposites (

To achieve semiconducting materials with high electron mobility in organic field-effect transistors (OFETs), low-lying energy levels (the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO)) and favorable molecular packing and ordering are two crucial factors. Here, it is reported that the incorporation of pyridine and selenophene into the backbone of a diketopyrrolopyrrole (DPP)-based copolymer produces a high-electron-mobility semiconductor, PDPPy-Se. Compared with analogous polymers based on other DPP derivatives and selenophene, PDPPy-Se features a lower LUMO that can decrease the electron transfer barrier for more effective electron injection, and simultaneously a lower HOMO that, however, can increase the hole transfer barrier to suppress the hole injection. Combined with thermal annealing at 240 °C for thin film morphology optimization to achieve large-scale crystallite domains with tight molecular packing for effective charge transport along the conducting channel, OFET devices fabricated with PDPPy-Se exhibit an n-type-dominant performance with an electron mobility (μe) as high as 2.22 cm2 V−1 s−1 and a hole/electron mobility ratio (μh/μe) of 0.26. Overall, this study demonstrates a simple yet effective approach to boost the electron mobility in organic transistors by synergistic use of pyridine and selenophene in the backbone of a DPP-based copolymer.

Owing to their potential of low-cost, low-temperature, environmentally-friendly manufacturability on stretchable and flexible substrates, organic semiconductor technology has already entered into our everyday life. Organic Field-Effect Transistors (OFETs) in particular are of interest for application in radio frequency identification tags, wearable electronics, sensors and OLED TVs and mobile devices, just to name a few. In order to make organic electronics an everyday reality, solution-processable high-mobility Donor-Acceptor type conjugated polymers such as P(NDI2OD-T2), BFS4 and PCDTPT, play a pivotal role. This thesis investigates the structure-function properties of such D-A co-polymers through a combination of OFET measurements and microstructural characterisation, the latter has carried out with synchrotron- and neutron-based techniques.

The charge transport and microstructural properties of five different molecular weight (MW) batches of the naphthalenediimide-thiophene copolymer P(NDI2OD-T2) are investigated. In particular, the field-effect transistor (FET) performance and thin-film microstructure of samples with MW varying from Mn = 10 to 41 kDa are studied. Unlike conventional semiconducting polymers such as poly(3-hexylthiophene) where FET mobility dramatically drops with decreasing molecular weight, the FET mobility of P(NDI2OD-T2)-based transistors processed from 1,2-dichlorobenzene is found to increase with decreasing MW. Using a combination of grazing-incidence wide-angle X-ray scattering, near-edge X-ray absorption fine-structure spectroscopy, atomic force microscopy, and resonant soft X-ray scattering, the increase in FET mobility with decreasing MW is attributed to the pronounced increase in the orientational correlation length (OCL) with decreasing MW. In particular, the OCL is observed to systematically increase from

An ambipolar organic field-effect transistor (OFET) based on poly(diketopyrrolopyrrole-terthiophene) (PDPPHD-T3) is shown by P. Sonar, H. Haick, and co-workers on page 4012 to sensitively detect xylene isomers at low to 40 ppm level in multiple sensing features. Combined with pattern-recognition algorithms, a sole ambipolar FET sensor, rather than arrays of sensors, is able to discriminate highly similar xylene structural isomers from each other.