Recent graphene research has triggered enormous interest in new two-dimensional ordered crystals constructed by the inclusion of elements other than carbon for bandgap opening. The design of new multifunctional two-dimensional materials with proper bandgap has become an important challenge. Here we report a layered two-dimensional network structure that possesses evenly distributed holes and nitrogen atoms and a C 2 N stoichiometry in its basal plane. The two-dimensional structure can be efficiently synthesized via a simple wetchemical reaction and confirmed with various characterization techniques, including scanning tunnelling microscopy. Furthermore, a field-effect transistor device fabricated using the material exhibits an on/off ratio of 10 7 , with calculated and experimental bandgaps of approximately 1.70 and 1.96 eV, respectively. In view of the simplicity of the production method and the advantages of the solution processability, the C 2 N-h2D crystal has potential for use in practical applications.

The formation of 2D polyaniline (PANI) has attracted considerable interest due to its expected electronic and optoelectronic properties. Although PANI was discovered over 150 y ago, obtaining an atomically well-defined 2D PANI framework has been a longstanding challenge. Here, we describe the synthesis of 2D PANI via the direct pyrolysis of hexaaminobenzene trihydrochloride single crystals in solid state. The 2D PANI consists of three phenyl rings sharing six nitrogen atoms, and its structural unit has the empirical formula of C 3 N. The topological and electronic structures of the 2D PANI were revealed by scanning tunneling microscopy and scanning tunneling spectroscopy combined with a first-principle density functional theory calculation. The electronic properties of pristine 2D PANI films (undoped) showed ambipolar behaviors with a Dirac point of -37 V and an average conductivity of 0.72 S/cm. After doping with hydrochloric acid, the conductivity jumped to 1.41 × 10 3 S/cm, which is the highest value for doped PANI reported to date. Although the structure of 2D PANI is analogous to graphene, it contains uniformly distributed nitrogen atoms for multifunctionality; hence, we anticipate that 2D PANI has strong potential, from wet chemistry to device applications, beyond linear PANI and other 2D materials.was discovered in 1834 (1), the word PANI was first coined in 1947 (2), and PANI garnered immense attention from the scientific community due to its intrinsically conducting nature (3). During the last three decades, PANI has been one of the most extensively studied conducting polymers because of its simple synthesis, low cost, high conductivity, environmental stability, and doping chemistry (4, 5). Linear PANI has found broad applicability in rechargeable batteries (6), electromagnetic shielding (7), nonlinear optics (8), light-emitting devices (9), sensors (10), field effect transistors (11), erasable optical information storage (12), membranes (13), digital memory devices (14) (27)], cyclic, spiral, and complex nanostructures have also been reported (28). However, due to the mechanistic complexity of aniline polymerization, the atomic-scale control of PANI structure has not yet been realized (28). Together with the recent discovery of all-carbon-based 2D graphene and its promising potentials (29), 2D network polymers are galvanizing a new wave of research in the scientific community (30). Here, we, for the first time to our knowledge, report the synthesis of real 2D PANI framework from direct pyrolysis of organic single crystals, hexaaminobenzene trihydrochloride (HAB), at 500°C. This synthetic methodology could serve as a straightforward way for the design and synthesis of other new 2D layered materials with many potential applications, from wet chemistry to devices. Results and DiscussionThe key building block, HAB, as a monomer with six functional groups (M6), was synthesized in a pure crystalline form (Fig. 1A and SI Appendix, Fig. S1) (31). It was observed that the HAB single crystals pyrolyze before mel...

Highly crystalline, phase- and size-controlled CoO nanocrystals of hexagonal and cubic phases have been prepared by thermal decomposition of Co(acac)3 in oleylamine under an inert atmosphere. Kinetic and thermodynamic control for the precursor formation leads to two different seeds of hexagonal and cubic phases at higher temperatures. The crystal size of both CoO phases can be easily manipulated by changing the precursor concentration and reaction temperature.

Recent interest in flexible electronics has led to a paradigm shift in consumer electronics, and the emergent development of stretchable and wearable electronics is opening a new spectrum of ubiquitous applications for electronics. Organic electronic materials, such as π-conjugated small molecules and polymers, are highly suitable for use in low-cost wearable electronic devices, and their charge-carrier mobilities have now exceeded that of amorphous silicon. However, their commercialization is minimal, mainly because of weaknesses in terms of operational stability, long-term stability under ambient conditions, and chemical stability related to fabrication processes. Recently, however, many attempts have been made to overcome such instabilities of organic electronic materials. Here, an overview is provided of the strategies developed for environmentally robust organic electronics to overcome the detrimental effects of various critical factors such as oxygen, water, chemicals, heat, and light. Additionally, molecular design approaches to π-conjugated small molecules and polymers that are highly stable under ambient and harsh conditions are explored; such materials will circumvent the need for encapsulation and provide a greater degree of freedom using simple solution-based device-fabrication techniques. Applications that are made possible through these strategies are highlighted.

The development of a versatile method for nitrogen-doping of graphitic structure is an important challenge for many applications, such as energy conversions and storages and electronic devices. Here, we report a simple but efficient method for preparing nitrogen-doped graphene nanoplatelets via wet-chemical reactions. The reaction between monoketone (C═O) in graphene oxide (GO) and monoamine-containing compound produces imine (Shiff base) functionalized GO (iGO). The reaction between α-diketone in GO and 1,2-diamine (ortho-diamine)-containing compound gives stable pyrazine ring functionalized GO (pGO). Subsequent heat-treatments of iGO and pGO result in high-quality, nitrogen-doped graphene nanoplatelets to be designated as hiGO and hpGO, respectively. Of particular interest, hpGO was found to display the n-type field-effect transistor behavior with a charge neutral point (Dirac point) located at around -16 V. Furthermore, hpGO showed hole and electron mobilities as high as 11.5 and 12.4 cm(2)V(-1)s(-1), respectively.

Highly flexible organic nanofiber phototransistors are fabricated on a highly flexible poly(ethylene terephthalate) (PET) textile/poly(dimethylsiloxane) (PDMS) composite substrate. Organic nanofibers are obtained by electrospinning, using a mixture of poly(3,3″′‐didodecylquarterthiophene) (PQT‐12) and poly(ethylene oxide) (PEO) as the semiconducting polymer and processing aid, respectively. PDMS is used as both a buffer layer for flattening the PET textile and a dielectric layer in the bottom‐gate bottom‐contact device configuration. PQT‐12:PEO nanofibers can be well‐aligned on the textile composite substrate by electrospinning onto a rotating drum collector. The nanofiber phototransistors fabricated on the PET/PDMS textile composite substrate show highly stable device performance (on‐current retention up to 82.3 (±6.7)%) under extreme bending conditions, with a bending radius down to 0.75 mm and repeated tests over 1000 cycles, while those prepared on film‐type PET and PDMS‐only substrates exhibit much poorer performances. The photoresponsive behaviors of PQT‐12:PEO nanofiber phototransistors have been investigated under light irradiation with different wavelengths. The maximum photoresponsivity, photocurrent/dark‐current ratio, and external quantum efficiency under blue light illumination were 930 mA W−1, 2.76, and 246%, respectively. Furthermore, highly flexible 10 × 10 photosensor arrays have been fabricated which are able to detect incident photonic signals with high resolution. The flexible photosensors described herein have high potential for applications as wearable photosensors.

Organic ambipolar transistor arrays for chemical sensors are prepared on a flexible plastic substrate with a bottom-gate bottom-contact configuration to minimize the damage to the organic semiconductors, for the first time, using a photolithographically patternable polymer semiconductor. Well-balanced ambipolar charge transport is achieved by introducing graphene electrodes because of the reduced contact resistance and energetic barrier for electron transport.

Phototransistors based on organic photoactive materials combine tunable light absorption in the spectral region from ultraviolet to near-infrared with low-temperature processability over large areas on flexible substrates. However, they often exhibit low photoresponsivity because of low molar extinction coefficient of photoactive components. We report a simple, yet highly efficient solution method for enhancing the performance of organic phototransistors using ruthenium complex 1 (Ru-complex 1). An air-stable n-type organic semiconductor, N,N'-bis(2-phenylethyl)-perylene-3,4:9,10-tetracarboxylic diimide (BPE-PTCDI), has been deposited on a silicon wafer and a transparent polyimide (PI) substrate via thermal evaporation under vacuum. The BPE-PTCDI phototransistors functionalized with Ru-complex 1 exhibit ∼5000 times higher external quantum efficiency (EQE) than that of pristine BPE-PTCDI phototransistors, owing to the metal-ligand charge transfer (MLCT) from Ru-complex 1 to the active component of the device. In addition, a large 10 × 10 phototransistor array (2.5 × 2.5 cm(2)) has been prepared on a transparent PI substrate, showing distinct light mapping. The fabricated phototransistor array is highly flexible and twistable and works well under tensile and compressive strains. We believe that our simple method will pave a viable way for improvements in the photoresponsivity of organic semiconductors for applications in wearable organic optoelectronic devices.