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Funder: Ministry of Science and Technology of the People’s Republic of China (Chinese Ministry of Science and Technology), The cornerstones of emerging high-performance organic photovoltaic devices are bulk heterojunctions, which usually contain both structure disorders and bicontinuous interpenetrating grain boundaries with interfacial defects. This feature complicates fundamental understanding of their working mechanism. Highly-ordered crystalline organic p–n heterojunctions with well-defined interface and tailored layer thickness, are highly desirable to understand the nature of organic heterojunctions. However, direct growth of such a crystalline organic p–n heterojunction remains a huge challenge. In this work, we report a design rationale to fabricate monolayer molecular crystals based p–n heterojunctions. In an organic field-effect transistor configuration, we achieved a well-balanced ambipolar charge transport, comparable to single component monolayer molecular crystals devices, demonstrating the high-quality interface in the heterojunctions. In an organic solar cell device based on the p–n junction, we show the device exhibits gate-tunable open-circuit voltage up to 1.04 V, a record-high value in organic single crystalline photovoltaics.

The instability of organic field-effect transistors (OFETs) is one key obstacle to practical application and is closely related to the unstable aggregate state of organic semiconductors (OSCs). However, the underlying reason for this instability remains unclear, and no effective solution has been developed. Herein, we find that the intrinsic tensile and compressive strains that exist in OSC films are the key origins for aggregate state instability and device degradation. We further report a strain balance strategy to stabilize the aggregate state by regulating film thickness, which is based on the unique transition from tensile strain to compressive strain with increasing film thickness. Consequently, a strain-free and ultrastable OSC film is obtained by regulating the film thickness, with which an ultrastable OFET with a five-year lifetime is realized. This work provides a deeper understanding of and a solution to the instability of OFETs and sheds light on their industrialization.

With the fast development of organic electronics, organic semiconductors have been extensively studied for various optoelectronic applications, among which organic phototransistors recently emerged as one of the most promising light signal detectors. However, it is still a big challenge to endow organic phototransistors with both high mobility and high light-sensitivity because the low mobility of most organic photoresponsive materials limits the efficiency of transporting and collecting charge carriers. We herein report band-like charge transport in vacuum-deposited small-molecule thin films for organic phototransistor arrays which can be operated at very low dark currents (~10−12 A). Both high mobility and excellent optical figures of merit including photosensitivity, photoresponsivity and detectivity are achieved, wherein, unprecedentedly, a detectivity greater than 1017 cm Hz1/2 W−1 is obtained. All these key parameters are superior to state-of-the-art organic phototransistors, implying a great potential in optoelectronic applications., The potential of organic phototransistors to surpass silicon-based devices is limited by the low carrier mobility of organic photoresponsive materials. Here, Ji et al. report high performance organic phototransistors featuring vacuum-deposited small-molecule films with band-like charge transport.

Integrating electronics and photonics is critically important for the realization of high-density and high-speed optoelectronic circuits. However, it remains challenging to achieve this target due to the difficulty of merging many different areas of science and technology. Here, we show an organic integrated optoelectronic device, namely, organic field-effect optical waveguide, integrating field-effect transistor and optical waveguide together. In such device, the propagation of optical waveguide in the active organic semiconductor can be tuned by the third terminal—the gate electrode of transistor, giving a controllable modulation depth as high as 70% and 50% in parallel and perpendicular directions of charge transport versus optical waveguide, respectively. Also, the optical waveguide with different directions can turn the field-effect of the device with the photodependence ratio up to 14800. The successful integration of active field-effect transistor with semiconductor waveguide modulator expands opportunities for creating scalable integration of electronics and photonics in a chip., Despite recent advances in organic optoelectronics development, integration of electronics and photonics in a chip remains a challenge. Here, the authors demonstrate organic field-effect optical waveguides that control propagating photons by the electric field produced in an organic transistor.

Integrating electronics and photonics is critically important for the realization of high-density and high-speed optoelectronic circuits. However, it remains challenging to achieve this target due to the difficulty of merging many different areas of science and technology. Here, we show an organic integrated optoelectronic device, namely, organic field-effect optical waveguide, integrating field-effect transistor and optical waveguide together. In such device, the propagation of optical waveguide in the active organic semiconductor can be tuned by the third terminal-the gate electrode of transistor, giving a controllable modulation depth as high as 70% and 50% in parallel and perpendicular directions of charge transport versus optical waveguide, respectively. Also, the optical waveguide with different directions can turn the field-effect of the device with the photodependence ratio up to 14800. The successful integration of active field-effect transistor with semiconductor waveguide modulator expands opportunities for creating scalable integration of electronics and photonics in a chip.

Self-assembly of monolayers of functional molecules on dielectric surfaces is a promising approach for the development of molecular devices proposed in the 1970s. Substrate chemically bonded self-assembled monolayers of semiconducting conjugated molecules exhibit low mobility. And self-assembled monolayer molecular crystals are difficult to scale up and limited to growth on substrates terminated by hydroxyl groups, which makes it difficult to realize sophisticated device functions, particularly for those relying on n-type electron transport, as electrons suffer severe charge trapping on hydroxyl terminated surfaces. Here we report a gravity-assisted, two-dimensional spatial confinement method for bottom-up growth of high-quality n-type single-crystalline monolayers over large, centimeter-sized areas. We demonstrate that by this method, n-type monolayer molecular crystals with high field-effect mobility of 1.24 cm2 V−1 s−1 and band-like transport characteristics can be grown on hydroxyl-free polymer surface. Furthermore, we used these monolayer molecular crystals to realize high-performance crystalline, gate-/light-tunable lateral organic p–n diodes., New methods for obtaining large-area monolayer molecular crystals (MMCs) on hydrophobic surfaces are needed to realize the full potential of MMCs for organic electronics. Here, the authors demonstrate bottom-up growth of high-grade n-type MMCs, which show superior performance in device applications.

The ever-increasing demand for flexible electronics calls for the development of low-voltage and high-mobility organic thin-film transistors (OTFTs) that can be integrated into emerging display and labeling technologies. Polymer dielectrics with comprehensive and balanced dielectric properties (i.e., a good balance between their insulating characteristics and compatibility with organic semiconductors) are considered particularly important for this end. Here, we introduce a simple but highly efficient strategy to realize this target by using a new type of copolymer as dielectrics. Benefiting from both high chain packing density guaranteeing dielectric properties and surface polarity optimizing molecular packing of organic semiconductors, this rationally designed copolymer dielectric endows flexible OTFTs with high mobility (5.6 cm2 V−1 s−1), low operating voltage (3 V) and outstanding stability. Further, their applicability in integrated circuits is verified. The excellent device performance shows exciting prospects of this molecular-scale engineered copolymer for the realization of plastic high-performance integrated electronics.

Molecular electronics describes a field that seeks to implement electronic components made of molecular building blocks. To date, few studies have used conjugated polymers in molecular junctions despite the fact that they potentially transport charge more efficiently than the extensively investigated small-molecular systems. Here we report a novel type of molecular tunnelling junction exploring the use of conjugated polymers, which are self-assembled into ultrathin films in a distinguishable ‘planar' manner from the traditional vertically oriented small-molecule monolayers. Electrical measurements on the junctions reveal molecular-specific characteristics of the polymeric molecules in comparison with less conjugated small molecules. More significantly, we decorate redox-active functionality into polymeric backbones, demonstrating a key role of redox centre in the modulation of charge transport behaviour via energy level engineering and external stimuli, and implying the potential of employing tailor-made polymeric components as alternatives to small molecules for future molecular-scale electronics., To date, conjugated polymers have not yet been used in molecular junctions despite the fact that they transport charge more efficiently than small-molecular systems. Here, Wang et al. showcase the self-assembly of conjugated polymers into ultrathin films in a planar manner for device construction.

Black phosphorus, a fast emerging two-dimensional material, has been configured as field effect transistors, showing a hole-transport-dominated ambipolar characteristic. Here we report an effective modulation on ambipolar characteristics of few-layer black phosphorus transistors through in situ surface functionalization with caesium carbonate (Cs2CO3) and molybdenum trioxide (MoO3), respectively. Cs2CO3 is found to strongly electron dope black phosphorus. The electron mobility of black phosphorus is significantly enhanced to similar to 27 cm(2)V(-1) s(-1) after 10 nm Cs2CO3 modification, indicating a greatly improved electron-transport behaviour. In contrast, MoO3 decoration demonstrates a giant hole-doping effect. In situ photoelectron spectroscopy characterization reveals significant surface charge transfer occurring at the dopants/black phosphorus interfaces. Moreover, the surface-doped black phosphorus devices exhibit a largely enhanced photodetection behaviour. Our findings coupled with the tunable nature of the surface transfer doping scheme ensure black phosphorus as a promising candidate for further complementary logic electronics.