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Abstract Despite recent dramatic improvements in the electronic characteristics of stretchable organic field-effect transistors (FETs), their low operational stability remains a bottleneck for their use in practical applications. Here, the operational stability, especially the bias-stress stability, of semiconducting polymer-based FETs under various tensile strains is investigated. Analyses on the structure of stretched semiconducting polymer films and spectroscopic quantification of trapped charges within them reveal the major cause of the strain-dependent bias-stress instability of the FETs. Devices with larger strains exhibit lower stability than those with smaller strains because of the increased water content, which is accompanied by the formation of cracks and nanoscale cavities in the semiconducting polymer film as results of the applied strain. The strain-dependence of bias-stress stability of stretchable OFETs can be eliminated by passivating the devices to avoid penetration of water molecules. This work provides new insights for the development of bias-stable stretchable OFETs.

Abstract Thermoelectric (TE) charge transport in organic TE nanocomposite systems is a critical consideration in designing high‐performance TE materials. Here, the relationship between the TE properties and energy structure of conducting polymer/quantum dot (QD) nanocomposites is systematically investigated by developing a potential wall or potential well in poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with CdTe QDs. The added QDs are primarily distributed within the electrically insulating PSS shell and act as stepping stones for charge transport between PEDOT‐rich grains. The embedded QDs generate an energy‐filtering effect, which is induced by both potential wall and potential well states established by the QDs in the PEDOT:PSS films. The induced energy‐filtering effect increases the Seebeck coefficient S with limited loss of electrical conductivity σ, thereby overcoming the TE trade‐off relation S ∝ σ −1/4. The energy‐filtering effect is optimized by carefully controlling the QD size. The PEDOT:PSS/QD nanocomposite containing the smallest QDs exhibits a power factor of 173.8 µW m−1 K−2, which is 80% larger than the value for the pristine PEDOT:PSS film. This work suggests a strategy for designing TE nanocomposites with improved TE performance and emphasizes the importance of fine‐tuning the interfacial energy gap to achieve an effective energy‐filtering effect.

Abstract The pressing demand for sustainable energy storage solutions has spurred the burgeoning development of aqueous zinc batteries. However, kinetics-sluggish Zn2+ as the dominant charge carriers in cathodes leads to suboptimal charge-storage capacity and durability of aqueous zinc batteries. Here, we discover that an ultrathin two-dimensional polyimine membrane, featured by dual ion-transport nanochannels and rich proton-conduction groups, facilitates rapid and selective proton passing. Subsequently, a distinctive electrochemistry transition shifting from sluggish Zn2+-dominated to fast-kinetics H+-dominated Faradic reactions is achieved for high-mass-loading cathodes by using the polyimine membrane as an interfacial coating. Notably, the NaV3O8·1.5H2O cathode (10 mg cm−2) with this interfacial coating exhibits an ultrahigh areal capacity of 4.5 mAh cm−2 and a state-of-the-art energy density of 33.8 Wh m−2, along with apparently enhanced cycling stability. Additionally, we showcase the applicability of the interfacial proton-selective coating to different cathodes and aqueous electrolytes, validating its universality for developing reliable aqueous batteries.

Abstract For organic solar cells to be competitive, the light-absorbing molecules should simultaneously satisfy multiple key requirements, including weak-absorption charge transfer state, high dielectric constant, suitable surface energy, proper crystallinity, etc. However, the systematic design rule in molecules to achieve the abovementioned goals is rarely studied. In this work, guided by theoretical calculation, we present a rational design of non-fullerene acceptor o-BTP-eC9, with distinct photoelectric properties compared to benchmark BTP-eC9. o-BTP-eC9 based device has uplifted charge transfer state, therefore significantly reducing the energy loss by 41 meV and showing excellent power conversion efficiency of 18.7%. Moreover, the new guest acceptor o-BTP-eC9 has excellent miscibility, crystallinity, and energy level compatibility with BTP-eC9, which enables an efficiency of 19.9% (19.5% certified) in PM6:BTP-C9:o-BTP-eC9 based ternary system with enhanced operational stability.

Abstract The water surface provides a highly effective platform for the synthesis of two-dimensional polymers (2DP). In this study, we present an efficient on-water surface synthesis of crystalline monolayer 2D polyimide (2DPI) through the imidization reaction between tetra (4-aminophenyl) porphyrin (M1) and perylenetracarboxylic dianhydride (M2), resulting in excellent stability and coverage over a large area (tens of cm2). We further fabricate innovative organic-inorganic hybrid van der Waals heterostructures (vdWHs) by combining with exfoliated few-layer molybdenum sulfide (MoS2). High-resolution transmission electron microscopy (HRTEM) reveals face-to-face stacking between MoS2 and 2DPI within the vdWH. This stacking configuration facilitates remarkable charge transfer and noticeable n-type doping effects from monolayer 2DPI to MoS2, as corroborated by Raman spectroscopy, photoluminescence measurements, and field-effect transistor (FET) characterizations. Notably, the 2DPI-MoS2 vdWH exhibits an impressive electron mobility of 50 cm2/V·s, signifying a substantial improvement over pristine MoS2 (8 cm2/V·s). This study unveils the immense potential of integrating 2D polymers to enhance semiconductor device functionality through tailored vdWHs, thereby opening up exciting new avenues for exploring unique interfacial physical phenomena.

Abstract Graphene is used as a growth template for van der Waals epitaxy of organic semiconductor (OSC) thin films. During the synthesis and transfer of chemical‐vapor‐deposited graphene on a target substrate, local inhomogeneities in the graphene—in particular, a nonuniform strain field in the graphene template—can easily form, causing poor morphology and crystallinity of the OSC thin films. Moreover, a strain field in graphene introduces a pseudo‐electric field in the graphene. Here, the study investigates how the strain and strain‐induced pseudo‐electric field of a graphene template affect the self‐assembly of π‐conjugated organic molecules on it. Periodically strained graphene templates are fabricated by transferring graphene onto an array of nanospheres and then analyzed the growth and nucleation behavior of C60 thin films on the strained graphene templates. Both experiments and a numerical simulation demonstrated that strained graphene reduced the desorption energy between the graphene and the C60 molecules and thereby suppressed both nucleation and growth of the C60. A mechanism is proposed in which the strain‐induced pseudo‐electric field in graphene modulates the binding energy of organic molecules on the graphene.

Abstract Interest has grown in services that consume a significant amount of energy, such as large language models (LLMs), and research is being conducted worldwide on synaptic devices for neuromorphic hardware. However, various complex processes are problematic for the implementation of synaptic properties. Here, synaptic characteristics are implemented through a novel method, namely side chain control of conjugated polymers. The developed devices exhibit the characteristics of the biological brain, especially spike‐timing‐dependent plasticity (STDP), high‐pass filtering, and long‐term potentiation/depression (LTP/D). Moreover, the fabricated synaptic devices show enhanced nonvolatile characteristics, such as long retention time (≈102 s), high ratio of Gmax/Gmin, high linearity, and reliable cyclic endurance (≈103 pulses). This study presents a new pathway for next‐generation neuromorphic computing by modulating conjugated polymers with side chain control, thereby achieving high‐performance synaptic properties.

Abstract The sequential deposition method assists the vertical phase distribution in the photoactive layer of organic solar cells, enhancing power conversion efficiencies. With this film coating approach, the morphology of both layers can be fine‐tuned with high boiling solvent additives, as frequently applied in one‐step casting films. However, introducing liquid additives can compromise the morphological stability of the devices due to the solvent residuals. Herein, 1,3,5‐tribromobenzene (TBB) with high volatility and low cost, is used as a solid additive in the acceptor solution and combined thermal annealing to regulate the vertical phase in organic solar cells composed of D18‐Cl/L8‐BO. Compared to the control cells, the devices treated with TBB and those that underwent additional thermal processing exhibit increased exciton generation rate, charge carrier mobility, charge carrier lifetime, and reduced bimolecular charge recombination. As a result, the TBB‐treated organic solar cells achieve a champion power conversion efficiency of 18.5% (18.1% averaged), one of the highest efficiencies in binary organic solar cells with open circuit voltage exceeding 900 mV. This study ascribes the advanced device performance to the gradient‐distributed donor‐acceptor concentrations in the vertical direction. The findings provide guidelines for optimizing the morphology of the sequentially deposited top layer to achieve high‐performance organic solar cells.

Abstract Conjugated polymer (CP)/carbon nanotube (CNT) composites have been actively used for thermoelectrics for more than a decade. Thermoelectric performance of CP/CNT composites is greatly improved compared with that of the individual components; however, the underlying origin of the performance improvement remains vague, without clear explanations at the molecular scale. Moreover, the nature of the heterogeneous system limits quantitative analysis and restricts physical understanding of the thermoelectric effect in the composites. By combining experimental approaches with molecular dynamics simulations, the contribution of the CPs to the thermoelectric properties at inter‐tube junctions between adjacent CNTs is revealed. Indacenodithiophene‐co‐benzothiadiazole (IDTBT), which has a highly planar backbone and does not aggregate at CP/CNT interfaces, can better mediate effective intramolecular charge transport along backbone chains at inter‐tube junctions than poly[2,5‐bis(3‐tetradecylthiophene‐2‐yl)thieno[3,2‐b]thiophene] (PBTTT). The isotropic and continuous distribution of IDTBT backbone chains enables both holes and phonons to be transported effectively at inter‐tube junctions; this effect greatly increases electrical conductivity, but also increases thermal conductivity. Thus, to obtain a high thermoelectric figure of merit, the balance between the two effects must be optimized. These results may enable CP/CNT composites, whose development is currently stagnating, to be developed into commercially available thermoelectrics, complementing their conventional inorganic counterparts.

Abstract Polymer semiconductors are promising materials for stretchable, wearable, and implantable devices due to their intrinsic flexibility, facile functionalization, and solution processability at low temperatures. However, the crystalline domain of the conjugated structure for high charge carrier mobility in semiconducting polymers exhibits lower stretchability than that of the semi‐crystalline or amorphous domains. Herein, a set of thermoplastic soft semiconductors is synthesized with different ratios of diketopyrrolopyrrole–carbazole–diketopyrrolopyrrole (DPP‐Cz‐DPP)‐based hard segments and thiophene‐based aliphatic soft segments, having the similar structure of thermoplastic elastomers. The polymers exhibit decreased glassy temperatures with the increased content of the soft segments. The polymers show high crystallinity after copolymerization with a large‐sized DPP‐Cz‐DPP core and non‐conjugated segments due to an aggregation property of the conjugated core, still possessing a semi‐crystalline domain after annealing. The polymer films exhibit stretchability under strains of up to 60%. Organic field‐effect transistors fabricated using stretchable polymers show a mobility range of 0.125–0.005 cm2 V−1 s−1 with different proportions of the soft segment. The stretchability is improved significantly and the mobilities are decreased less when the content of the soft segment is increased. Therefore, this study presents a design principle for the development of a high‐performance stretchable semiconducting polymer.

Though skin-attachable vibration sensors are promising for voice recognition applications, current technologies do not meet key performance requirements. Here, the authors report a flexible skin-attachable sensor with high sensitivity and flat frequency response over the vocal frequency range.

The scalability of printable integrated circuits is lagging far behind that of conventional silicon-based technologies. Here, Kwon et al. show a three-dimensional integration approach by stacking printeddual-gate organic transistors on plastic foils with a density of 60 transistors per centimeter square.

Abstract Human skin plays a critical role in a person communicating with his or her environment through diverse activities such as touching or deforming an object. Various electronic skin (E‐skin) devices have been developed that show functional or geometrical superiority to human skin. However, research into stretchable E‐skin that can simultaneously distinguish materials and textures has not been established yet. Here, the first approach to achieving a stretchable multimodal device is reported, that operates on the basis of various electrical properties of piezoelectricity, triboelectricity, and piezoresistivity and that exceeds the capabilities of human tactile perception. The prepared E‐skin is composed of a wrinkle‐patterned silicon elastomer, hybrid nanomaterials of silver nanowires and zinc oxide nanowires, and a thin elastomeric dielectric layer covering the hybrid nanomaterials, where the dielectric layer exhibits high surface roughness mimicking human fingerprints. This versatile device can identify and distinguish not only mechanical stress from a single stimulus such as pressure, tensile strain, or vibration but also that from a combination of multiple stimuli. With simultaneous sensing and analysis of the integrated stimuli, the approach enables material discrimination and texture recognition for a biomimetic prosthesis when the multifunctional E‐skin is applied to a robotic hand.

Abstract User‐interactive electronic skin (e‐skin) with a distinguishable output has enormous potential for human–machine interfaces and healthcare applications. Despite advances in user‐interactive e‐skins, advances in visual user‐interactive therapeutic e‐skins remain rare. Here, a user‐interactive thermotherapeutic device is reported that is fabricated by combining thermochromic composites and stretchable strain sensors consisting of strain‐responsive silver nanowire networks on surface energy‐patterned microwrinkles. Both the color and heat of the device are easily controlled through electrical resistance variation induced by applied mechanical strain. The resulting monolithic device exhibits substantial changes in optical reflectance and temperature with durability, rapid response, high stretchability, and linear sensitivity. The approach enables a low‐expertise route to fabricating dynamic interactive thermotherapeutic e‐skins that can be used to effectively rehabilitate injured connective tissues as well as to prevent skin burns by simultaneously accommodating stretching, providing heat, and exhibiting a color change.

Abstract Controlling the growth behavior of organic semiconductors (OSCs) is essential because it determines their optoelectronic properties. In order to accomplish this, graphene templates with electronic‐state tunability are used to affect the growth of OSCs by controlling the van der Waals interaction between OSC ad‐molecules and graphene. However, in many graphene‐molecule systems, the charge transfer between an ad‐molecule and a graphene template causes another important interaction. This charge‐transfer‐induced interaction is never considered in the growth scheme of OSCs. Here, the effects of charge transfer on the formation of graphene–OSC heterostructures are investigated, using fullerene (C60) as a model compound. By in situ electrical doping of a graphene template to suppress the charge transfer between C60 ad‐molecules and graphene, the layer‐by‐layer growth of a C60 film on graphene can be achieved. Under this condition, the graphene–C60 interface is free of Fermi‐level pinning; thus, barristors fabricated on the graphene–C60 interface show a nearly ideal Schottky–Mott limit with efficient modulation of the charge‐injection barrier. Moreover, the optimized C60 film exhibits a high field‐effect electron mobility of 2.5 cm2 V−1 s−1. These results provide an efficient route to engineering highly efficient optoelectronic graphene–OSC hybrid material applications.

Abstract Utilizing the intrinsic mobility–strain relationship in semiconductors is critical for enabling strain engineering applications in high‐performance flexible electronics. Here, measurements of Hall effect and Raman spectra of an organic semiconductor as a function of uniaxial mechanical strain are reported. This study reveals a very strong, anisotropic, and reversible modulation of the intrinsic (trap‐free) charge carrier mobility of single‐crystal rubrene transistors with strain, showing that the effective mobility of organic circuits can be enhanced by up to 100% with only 1% of compressive strain. Consistently, Raman spectroscopy reveals a systematic shift of the low‐frequency Raman modes of rubrene to higher (lower) frequencies with compressive (tensile) strain, which is indicative of a reduction (enhancement) of thermal molecular disorder in the crystal with strain. This study lays the foundation of the strain engineering in organic electronics and advances the knowledge of the relationship between the carrier mobility, low‐frequency vibrational modes, strain, and molecular disorder in organic semiconductors.

Abstract The excitation intensity dependent carrier dynamics of blends with PC[70]BM of three new medium-band gap conjugated polymers with central chalcogen heteroatoms, PBDTfDTBX (X = O, T(Sulphur), Se) were studied. The PBDTfDTBX polymers (Poly[4,8-bis(5-(2-butyloctyl)thiophene-2-yl)benzo[1,2-b;4,5-b′]dithiophene-alt-4,7-bis(4-(2-ethylhexyl)-2-thienyl)-dithieno[3′,2′:3,4;2″,3″:5,6]benzo[1,2-c][1,2,5] furazan or thiadiazole or selenadiazole]) have symmetrical structures but exhibit different solar cell performances. In this study, we determined how the photogenerated charge carrrier dynamics of the PBDTfDTBX:PC[70]BM blends varies with the heteroatom by performing transient absorption measurements at various excitation intensities. It was found that the charge carrier dynamics of the PBDTfDTBX blends with X = T or Se heteroatoms are dependent on the excitation intensity whereas that of the PBDTfDTBO blend is independent of the intensity. The photogenerated charge carrier dynamics of the PBDTfDTBO:PCBM, PBDTfDTBT:PCBM, and PBDTfDTBSe:PCBM blends were all modeled globally and rates were estimated for different photophysical processes occurring on different time scales.