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The organic photodiode (OPD) is a promising building block for solution‐processable, flexible, lightweight, and miniaturized photodetectors, ideal for wearable applications. Despite the advances in materials used in OPDs, their photocurrent and light responsivity are limited, and alternative methods are required to boost the signal response. Herein, a miniaturized organic electrochemical transistor (OECT) is integrated with an OPD module to unlock the potential of OPDs to acquire physiological signals. In this integrated photodetector (IPD) system, the light intensity regulates the OPD voltage output that modulates the OECT channel current. The high transconductance of the OECT provides efficient voltage‐to‐current conversion, enhancing the signal‐to‐noise ratio on the sensing site. A microscale, p‐type enhancement‐mode OECT with high gm and fast switching speed performs better in this application than depletion‐mode OECT of the same geometry. The IPD achieves a photocurrent and responsivity 318 and 140 times higher than the standalone OPD, respectively. It is shown that with the IPD, the amplitude of the photoplethysmogram signals detected by the OPD is enhanced by a factor of 2.9 × 103, highlighting its potential as a wearable biosensor and to detect weak, often uncaptured, light‐based signals from living systems. [ABSTRACT FROM AUTHOR]

Slot‐die (SD) coating is used to fabricate fully solution processed organic solar cells (OSCs) based on a blend of high performance donor polymer (PTB7‐Th) and a non‐fullerene acceptor (IEICO‐4F) for stable devices over extended periods of operation. The optimization of a sequential deposition process of transport and active layers, under ambient conditions, enable high efficiency slot‐die coated solar cells with remarkable power conversion efficiencies (PCE) > 11.0% to bridge the gap between lab‐to‐fab. Fully slot‐die coated inverted OSCs are demonstrated with efficiencies reaching 11% along with 1 cm2 devices, proving the scalability and reproducibility of the proposed technique. Further, replacing the evaporated Ag electrode with solution processed Ag nanowire (AgNW) electrodes shows the highest light utilization efficiency of 5.26% for semi‐transparent OSC with a PCE of 9.07% and average visible transmission of 58%. [ABSTRACT FROM AUTHOR]

New polymer donors and nonfullerene acceptors have elevated the performance and stability of solar cells to higher grounds. To achieve their full potential, they require their adaptation to scalable and cost‐effective solution manufacturing techniques for large area deposition. Likewise, formulating scalable solution‐based transport layer inks that are compatible with the photoactive layer is imperative. This manuscript reports the full integration of solution‐based transport layers and electrode alongside a PTB7‐Th:IEICO‐4F bulk heterojunction in inverted architecture through inkjet‐printing, resulting in power conversion efficiencies up to 12.4% opaque devices and 9.5% semitransparent devices with average visible transmittance values of 50.1%, including hole transport layer. The wetting envelope of the highly‐hydrophobic photoactive layer alongside the surface energy of candidate solutions and solvents allows the formulation of thick transport layer inks that are compatible with the drop‐on‐demand inkjet‐printing process and yield uniform and homogenous films. Moreover, the surface energy components of the donor and acceptor serves as a fingerprint to assess the vertical stratification of the photoactive layer with the inclusion of different solvents. This methodology addresses a scale‐up bottleneck of solution‐based transport layers for high‐efficiency organic cells, enabling its adaptation to high‐throughput techniques including slot‐die and roll‐to‐roll coating. [ABSTRACT FROM AUTHOR]

While photovoltaic blends based on non‐fullerene acceptors are touted for their thermal stability, this type of acceptor tends to crystallize, which can result in a gradual decrease in photovoltaic performance and affects the reproducibility of the devices. Two halogenated indacenodithienothiophene‐based acceptors that readily co‐crystallize upon mixing are studied, which indicates that the use of an acceptor mixture alone does not guarantee the formation of a disordered mixture. The addition of the donor polymer to the acceptor mixture readily suppresses the crystallization, which results in a fine‐grained ternary blend with nanometer‐sized domains that do not coarsen due to a high Tg ≈ 200 °C. As a result, annealing at temperatures of up to 170 °C does not markedly affect the photovoltaic performance of ternary devices, in contrast to binary devices that suffer from acceptor crystallization in the active layer. The results indicate that the ternary approach enables the use of high‐temperature processing protocols, which are needed for upscaling and high‐throughput fabrication of organic solar cells. Further, ternary devices display a stable photovoltaic performance at 130 °C for at least 205 h, which indicates that the use of acceptor mixtures allows to fabricate devices with excellent thermal stability. [ABSTRACT FROM AUTHOR]

Power conversion efficiencies of perovskite solar cells (PSCs) have rapidly increased from 3.8% to a certified 25.2% within only a decade. Eliminating possible recombination losses at the interfaces is essential to further improve both efficiency and stability of this class of emerging photovoltaic technology. Herein, a simple approach for improving the electron extraction of the PC60BM electron transport layer (ETL) is presented by sequentially depositing Al:ZnO (AZO) and triphenyl‐phosphine oxide (TPPO) on top of it, in a p–i–n device configuration. The efficiency of the resulting CH3NH3PbI3‐based solar cell is shown to improve from 14.6%, measured for the control PC60BM‐only cell, to 17.9% for double‐ETL (PC60BM/AZO) and 19.2% for triple‐ETL (PC60BM/AZO/TPPO)‐based devices, respectively. Optimized triple‐ETL‐based cells exhibit high fill factor of 82%. The combination of electrical and quantum mechanical calculations shows that efficiency improvement is attributed to reduced trap‐assisted recombination at the interface and better energy level alignment due to chemical interactions between PC60BM, AZO, and TPPO. Moreover, it is shown that the use of multilayer ETL results in better device stability (T80 ≈ 800 h) under constant illumination. This work opens new possibilities for inexpensive highly efficient and stable multilayered contacts for PSCs by combining organic small molecules and metal oxides. [ABSTRACT FROM AUTHOR]

Abstract: N‐type organic small molecules (SMs) are attracting attention in the organic electronics field, due to their easy purification procedures with high yield. However, only a few reports show SMs that perform well in both organic field‐effect transistors (OFETs) and organic solar cells (OSCs). Here, the synthesis and characterization of an n‐type small molecule with an indacenodithieno[3,2‐b]thiophene (IDTT) core unit and linear alkylated side chain (C16) (IDTTIC) are reported. Compared to the state‐of‐the‐art n‐type molecule IDTIC, IDTTIC exhibits smaller optical bandgap and higher absorption coefficient, which is due to the enhanced intramolecular effect. After mixing with the polymer donor PBDB‐T, IDTIC‐based solar cells deliver a power conversion efficiency of only 5.67%. In stark contrast, the OSC performance of IDTTIC improves significantly to 11.2%. It is found that the superior photovoltaic properties of PBDB‐T:IDTTIC blends are mainly due to reduced trap‐assisted recombination and enhanced molecular packing coherence length and higher domain purity when compared to IDTIC. Moreover, a significantly higher electron mobility of 0.50 cm2 V−1 s−1 for IDTTIC in OFET devices than for IDTIC (0.15 cm2 V−1 s−1) is obtained. These superior performances in OSCs and OFETs demonstrate that SMs with extended π‐conjugation of the backbone possess a great potential for application in organic electronic devices. [ABSTRACT FROM AUTHOR]

Abstract: Nonfullerene acceptors (NFAs) in blends with highly crystalline donor polymers have been shown to yield particularly high device voltage outputs, but typically more modest quantum yields for photocurrent generation as well as often lower fill factors (FF). In this study, we employ transient optical and optoelectronic analysis to elucidate the factors determining device photocurrent and FF in blends of the highly crystalline donor polymer PffBT4T‐2OD with the promising NFA FBR or the more widely studied fullerene acceptor PC71BM. Geminate recombination losses, as measured by ultrafast transient absorption spectroscopy, are observed to be significantly higher for PffBT4T‐2OD:FBR blends. This is assigned to the smaller LUMO‐LUMO offset of the PffBT4T‐2OD:FBR blends relative to PffBT4T‐2OD:PC71BM, resulting in the lower photocurrent generation efficiency obtained with FBR. Employing time delayed charge extraction measurements, these geminate recombination losses are observed to be field dependent, resulting in the lower FF observed with PffBT4T‐2OD:FBR devices. These data therefore provide a detailed understanding of the impact of acceptor design, and particularly acceptor energetics, on organic solar cell performance. Our study concludes with a discussion of the implications of these results for the design of NFAs in organic solar cells. [ABSTRACT FROM AUTHOR]

The photovoltaic performance and optoelectronic properties of a donor-acceptor copolymer are reported based on indacenodithienothiophene (IDTT) and 2,3-bis(3-(octyloxy)phenyl)quinoxaline moieties (PIDTTQ) as a function of the number-average molecular weight ( Mn). Current-voltage measurements and photoinduced charge carrier extraction by linear increasing voltage (photo-CELIV) reveal improved charge generation and charge transport properties in these high band gap systems with increasing Mn, while polymers with low molecular weight suffer from diminished charge carrier extraction because of low mobility-lifetime ( μτ) product. By combining Fourier-transform photocurrent spectroscopy (FTPS) with electroluminscence spectroscopy, it is demonstrate that increasing Mn reduces the nonradiative recombination losses. Solar cells based on PIDTTQ with Mn = 58 kD feature a power conversion efficiency of 6.0% and a charge carrier mobility of 2.1 × 10−4 cm2 V−1 s−1 when doctor bladed in air, without the need for thermal treatment. This study exhibits the strong correlations between polymer fractionation and its optoelectronics characteristics, which informs the polymer design rules toward highly efficient organic solar cells. [ABSTRACT FROM AUTHOR]

With the advent of flexible and wearable electronics and sensors, there is an urgent need to develop energy‐harvesting solutions that are compatible with such wearables. However, many of the proposed energy‐harvesting solutions lack the necessary mechanical properties, which make them susceptible to damage by repetitive and continuous mechanical stresses, leading to serious degradation in device performance. Developing new energy materials that possess high deformability and self‐healability is essential to realize self‐powered devices. Herein, a thermoelectric ternary composite is demonstrated that possesses both self‐healing and stretchable properties produced via 3D‐printing method. The ternary composite films provide stable thermoelectric performance during viscoelastic deformation, up to 35% tensile strain. Importantly, after being completely severed by cutting, the composite films autonomously recover their thermoelectric properties with a rapid response time of around one second. Using this self‐healable and solution‐processable composite, 3D‐printed thermoelectric generators are fabricated, which retain above 85% of their initial power output, even after repetitive cutting and self‐healing. This approach represents a significant step in achieving damage‐free and truly wearable 3D‐printed organic thermoelectrics. [ABSTRACT FROM AUTHOR]

High fill factors have only recently become commonplace in nonfullerene‐based organic solar cells, with the balance of charge carrier mobilities often cited as the contributing factor. Here an end‐group modification to a commonly used nonfullerene acceptor (O‐IDTBR) is reported, in which the rhodanine end groups are replaced with dicyano moieties, resulting in the acceptor O‐IDTBCN. This new acceptor affords significant improvement in the fill factor (73%) and photocurrent (19.8 mA cm−2) in organic solar cells with the low bandgap polymer PTB7‐Th. A narrowing of the bandgap, as a result of greater push–pull hybridization, allows complementary absorption to the donor and thus improved photon harvesting. Additionally, the measurement of charge carrier mobilities and lifetimes in both systems reveal that the PTB7‐Th:O‐IDTBCN blend possesses more balanced charge carrier mobilities, and longer lifetimes. Morphology studies reveal a slightly greater degree of molecular mixing of the O‐IDTBCN when blended with PTB7‐Th, despite the greater and more balanced charge carrier mobilities in this blend. [ABSTRACT FROM AUTHOR]

Molecular orientation and π–π stacking of nonfullerene acceptors (NFAs) determine its domain size and purity in bulk‐heterojunction blends with a polymer donor. Two novel NFAs featuring an indacenobis(dithieno[3,2‐b:2ʹ,3ʹ‐d]pyrrol) core with meta‐ or para‐alkoxyphenyl sidechains are designed and denoted as m‐INPOIC or p‐INPOIC, respectively. The impact of the alkoxyl group positioning on molecular orientation and photovoltaic performance of NFAs is revealed through a comparison study with the counterpart (INPIC‐4F) bearing para‐alkylphenyl sidechains. With inward constriction toward the conjugated backbone, m‐INPOIC presents predominant face‐on orientation to promote charge transport. The as‐cast organic solar cells (OSCs) by blending m‐INPOIC and PBDB‐T as active layers exhibit a power conversion efficiency (PCE) of 12.1%. By introducing PC71BM as the solid processing‐aid, the ternary OSCs are further optimized to deliver an impressive PCE of 14.0%, which is among the highest PCEs for as‐cast single‐junction OSCs reported in literature to date. More attractively, PBDB‐T:m‐INPOIC:PC71BM based OSCs exhibit over 11% PCEs even with an active layer thickness over 300 nm. And the devices can retain over 95% of PCE after storage for 20 days. The outstanding tolerance to film thickness and outstanding stability of the as‐cast devices make m‐INPOIC a promising candidate NFA for large‐scale solution‐processable OSCs. [ABSTRACT FROM AUTHOR]

The high crystallinity and ability to harvest near‐infrared photons make diketopyrrolopyrrole (DPP)‐based polymers one of the most promising donors for high performing organic solar cells (OSCs). However, DPP‐based OSC devices still suffer from the trade‐off between energetic loss (Eloss) and maximum external quantum efficiency (EQEmax), which significantly hinders their potential. Thus far, the replacement of fullerenes with small molecule acceptors did not wisdom the performance development of DPP‐donor‐based solar cells due to severe charge recombination issues. In this work, efficient DPP‐based solar cells are reported using low bandgap fused ring electron acceptor, IEICO‐4F. PBDTT‐DPP:IEICO‐4F OSC devices deliver a champion power conversion efficiency of 9.66% with successful interface engineering along with low Eloss of 0.57 eV and a high EQEmax (>70%). [ABSTRACT FROM AUTHOR]

Organic–inorganic hybrid materials are of significant interest owing to their diverse applications ranging from photovoltaics and electronics to catalysis. Control over the organic and inorganic components offers flexibility through tuning their chemical and physical properties. Herein, it is reported that a new organic–inorganic hybrid, [Mn(C2H6OS)6]I4, with linear tetraiodide anions exhibit an ultralow thermal conductivity of 0.15 ± 0.01 W m−1 K−1 at room temperature, which is among the lowest values reported for organic–inorganic hybrid materials. Interestingly, the hybrid compound has a unique 0D structure, which extends into 3D supramolecular frameworks through nonclassical hydrogen bonding. Phonon band structure calculations reveal that low group velocities and localization of vibrational energy underlie the observed ultralow thermal conductivity, which could serve as a general principle to design novel thermal management materials. Intriguing physical and chemical properties of a 0D organic–inorganic hybrid crystal lead to unique thermal transport. Ultralow thermal conducti‐vity of 0.15 W m−1 K−1 is recorded for [Mn(C2H6OS)6]I4 owing to its 0D structure and localization of vibrational energy. [ABSTRACT FROM AUTHOR]