The communication outposts of the emerging Internet of Things are embodied by ordinary items, which desirably include all-printed flexible sensors, actuators, displays and akin organic electronic interface devices in combination with silicon-based digital signal processing and communication technologies. However, hybrid integration of smart electronic labels is partly hampered due to a lack of technology that (de)multiplex signals between silicon chips and printed electronic devices. Here, we report all-printed 4-to-7 decoders and seven-bit shift registers, including over 100 organic electrochemical transistors each, thus minimizing the number of terminals required to drive monolithically integrated all-printed electrochromic displays. These relatively advanced circuits are enabled by a reduction of the transistor footprint, an effort which includes several further developments of materials and screen printing processes. Our findings demonstrate that digital circuits based on organic electrochemical transistors (OECTs) provide a unique bridge between all-printed organic electronics (OEs) and low-cost silicon chip technology for Internet of Things applications.

Organic electrochemical transistors (OECTs) hold promise for developing a variety of high‐performance (bio‐)electronic devices/circuits. While OECTs based on p‐type semiconductors have achieved tremendous progress in recent years, n‐type OECTs still suffer from low performance, hampering the development of power‐efficient electronics. Here, it is demonstrated that fine‐tuning the molecular weight of the rigid, ladder‐type n‐type polymer poly(benzimidazobenzophenanthroline) (BBL) by only one order of magnitude (from 4.9 to 51 kDa) enables the development of n‐type OECTs with record‐high geometry‐normalized transconductance (gm,norm ≈ 11 S cm−1) and electron mobility × volumetric capacitance (µC* ≈ 26 F cm−1 V−1 s−1), fast temporal response (0.38 ms), and low threshold voltage (0.15 V). This enhancement in OECT performance is ascribed to a more efficient intermolecular charge transport in high‐molecular‐weight BBL than in the low‐molecular‐weight counterpart. OECT‐based complementary inverters are also demonstrated with record‐high voltage gains of up to 100 V V−1 and ultralow power consumption down to 0.32 nW, depending on the supply voltage. These devices are among the best sub‐1 V complementary inverters reported to date. These findings demonstrate the importance of molecular weight in optimizing the OECT performance of rigid organic mixed ionic–electronic conductors and open for a new generation of power‐efficient organic (bio‐)electronic devices.

Conducting polymers, such as the p-doped poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have enabled the development of an array of opto- and bio-electronics devices. However, to make these technologies truly pervasive, stable and easily processable, n-doped conducting polymers are also needed. Despite major efforts, no n-type equivalents to the benchmark PEDOT:PSS exist to date. Here, we report on the development of poly(benzimidazobenzophenanthroline):poly(ethyleneimine) (BBL:PEI) as an ethanol-based n-type conductive ink. BBL:PEI thin films yield an n-type electrical conductivity reaching 8 S cm−1, along with excellent thermal, ambient, and solvent stability. This printable n-type mixed ion-electron conductor has several technological implications for realizing high-performance organic electronic devices, as demonstrated for organic thermoelectric generators with record high power output and n-type organic electrochemical transistors with a unique depletion mode of operation. BBL:PEI inks hold promise for the development of next-generation bioelectronics and wearable devices, in particular targeting novel functionality, efficiency, and power performance.

Future brain-machine interfaces, prosthetics, and intelligent soft robotics will require integrating artificial neuromorphic devices with biological systems. Due to their poor biocompatibility, circuit complexity, low energy efficiency, and operating principles fundamentally different from the ion signal modulation of biology, traditional Silicon-based neuromorphic implementations have limited bio-integration potential. Here, we report the first organic electrochemical neurons (OECNs) with ion-modulated spiking, based on all-printed complementary organic electrochemical transistors. We demonstrate facile bio-integration of OECNs with Venus Flytrap (Dionaea muscipula) to induce lobe closure upon input stimuli. The OECNs can also be integrated with all-printed organic electrochemical synapses (OECSs), exhibiting short-term plasticity with paired-pulse facilitation and long-term plasticity with retention >1000 s, facilitating Hebbian learning. These soft and flexible OECNs operate below 0.6 V and respond to multiple stimuli, defining a new vista for localized artificial neuronal systems possible to integrate with bio-signaling systems of plants, invertebrates, and vertebrates.

In this paper, (1) a simple and controllable method to synthesize single crystalline nanoribbons of CuTCNQ in a large area was demonstrated by using a physical and chemical vapor combined deposition technique. (2) Nanoribbons synthesized by this method were identified to belong to phase I. (3) Devices and device arrays of nanoribbons were in situ fabricated by this method using gap electrodes and gap electrode arrays. (4) Current-voltage characteristics of crystalline devices and device arrays of nanoribbons exhibited semiconductor properties, and this conclusion was further confirmed by the results of devices based on an individual nanoribbon or microribbon of CuTCNQ (phase I). The controllable synthesis of nanoribbons for the in situ fabrication of crystalline nanodevices and device arrays will be attractive for nanoelectronics. Moreover, semiconductor current-voltage characteristics of the nanoribbons will be beneficial to the understanding of CuTCNQ.

We report on single nanofiber field-effect transistors made by the light-emitting polymer, poly(2-methoxy-5-(2-ethylhexoxy)-1,4-phenylenevinylene). We measure electrical performances comparable to or better than those of thin-film transistors by the same organic semiconductor, due to the molecular alignment induced by electrospinning, such as hole mobility of the order of 10(-3) cm(2) V(-1) s(-1) and on/off current ratios up to 780. In addition, we observe controllable photoluminescence intensity quenching by varying the gate voltage up to -40 V with device operation in the luministor mode. Single light-emitting polymer nanofiber transistors coupling electrical and optical functionalities open the way towards low cost and flexible one-dimensional switches and nanofiber-based light-emitting transistors.

Vertical organic electrochemical transistors (OECTs) have been manufactured solely using screen printing. The OECTs are based on PEDOT:PSS (poly(3,4-ethylenedioxythiophene) doped with poly (styrene sulfonic acid)), which defines the active material for both the transistor channel and the gate electrode. The resulting vertical OECT devices and circuits exhibit low-voltage operation, relatively fast switching, small footprint and high manufacturing yield; the last three parameters are explained by the reliance of the transistor configuration on a robust structure in which the electrolyte vertically bridges the bottom channel and the top gate electrode. Two different architectures of the vertical OECT have been manufactured, characterized and evaluated in parallel throughout this report. In addition to the experimental work, SPICE models enabling simulations of standalone OECTs and OECT-based circuits have been developed. Our findings may pave the way for fully integrated, lowvoltage operating and printed signal processing systems integrated with e.g. printed batteries, solar cells, sensors and communication interfaces. Such technology can then serve a low-cost base technology for the internet of things, smart packaging and home diagnostics applications.

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