Flexible neuromorphic electronics that emulate biological neuronal systems constitute a promising candidate for next‐generation wearable computing, soft robotics, and neuroprosthetics. For realization, with the achievement of simple synaptic behaviors in a single device, the construction of artificial synapses with various functions of sensing and responding and integrated systems to mimic complicated computing, sensing, and responding in biological systems is a prerequisite. Artificial synapses that have learning ability can perceive and react to events in the real world; these abilities expand the neuromorphic applications toward health monitoring and cybernetic devices in the future Internet of Things. To demonstrate the flexible neuromorphic systems successfully, it is essential to develop artificial synapses and nerves replicating the functionalities of the biological counterparts and satisfying the requirements for constructing the elements and the integrated systems such as flexibility, low power consumption, high‐density integration, and biocompatibility. Here, the progress of flexible neuromorphic electronics is addressed, from basic backgrounds including synaptic characteristics, device structures, and mechanisms of artificial synapses and nerves, to applications for computing, soft robotics, and neuroprosthetics. Finally, future research directions toward wearable artificial neuromorphic systems are suggested for this emerging area.

properties of biological synapses and perform parallel operations, they require larger energy than a biological synapse. Therefore, development of an artificial synapse with energy consumption on the level of a biological synapse remains an open problem.Organic-inorganic halide perovskite (OHPs) may provide a material to solve this problem, because of their low activation energy of ion migration. Moreover, various structural modulation of polycrystalline films is possible with facile solution processing so that organic parts in the OHPs can control the ion migration and electrical conduction. OHPs have an ABX 3 crystal structure; the A-site cation is located at the center of a BX 6 octahedral cage, and the B-site metal cation is surrounded by the six nearest-neighbor X-site halide anions. [7] OHPs have a significant hysteresis property that is caused by ion migration or space charges, or both, which may enable gradual modulation of conductance in OHP. [8] Two-terminal artificial synapses based on 3D methylammonium (MA) lead halide perovskite (MAPbX 3 , X = Br, I) films showed synaptic responses that are caused by ion migration in the OHP layer. [9,10] Ion migration in 3D OHP film is induced by relatively low activation energy and a low energy consumption of ≈20 fJ per synaptic event was achieved in the synaptic devices. However, the energy consumption could be further reduced to the energy level of biological synapses when the ion migration was controlled by engineering the structure of OHP films could be optimally done.In this work, we introduce 2D and quasi-2D OHP films into artificial synapses to enable control of ion migration and resultant synaptic responses. For this purpose, we replaced the small MA ion with a bulky phenethylammonium (PEA) ion in their crystalline structures. To prepare 2D, quasi-2D, and 3D OHP films, we controlled the stoichiometric ratio of PEA and MA cations to induce self-assembly of a layered structure. This replacement of an MA cation with PEA cation suppresses ion migration in the out-of-plane direction of the OHP films. [11][12][13] Thereby, the activation energy E A of ion migration is increased, so ion migration and excitatory postsynaptic current (EPSC) can be reduced. Also, energy consumption of the device is reduced to ≈0.7 fJ per synaptic event, which is comparable to that of biological synapses. Memory retention of artificial The hysteretic behavior of organic-inorganic halide perovskites (OHPs) are exploited for application in neuromorphic electronics. Artificial synapses with 2D and quasi-2D perovskite are demonstrated that have a bulky organic cation (phenethylammonium (PEA)) to form structures of (PEA) 2 MA n-1 Pb n Br 3n+1 . The OHP films have morphological properties that depend on their structure dimensionality (i.e., n value), and artificial synapses fabricated from them show synaptic responses such as short-term plasticity, paired-pulse facilitation, and long-term plasticity. The operation mechanism of OHP artificial synapses are also analyzed depending on the dimen...

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Organic synaptic transistors using intrinsic (i.e., non‐doped) organic semiconductors have demonstrated various synaptic functions to mimic biological synapses, but the devices show limited long‐term retention behaviors although long‐term memory is essential for neuromorphic computing. To achieve long‐term retention time, correlating the synaptic responses with the microstructures of polymer semiconductor is an imperative step. It is shown that synaptic plasticity in ion‐gel‐gated organic synaptic transistors (IGOSTs) can be modulated by controlling the microstructure of organic semiconductors and that long‐term memory retention can be significantly prolonged by increasing their crystallinity. The crystallinity of poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) films that are spun‐cast on bare and self‐assembled monolayer is systematically controlled, before and after thermal treatments. Long‐term retention tends to extend, as the crystallinity increases. To evaluate synaptic current decay behaviors, it is suggested that the relaxation is a result of de‐doping of the polymer semiconductor over time. The recognition of handwritten digits is simulated and a high classification accuracy (>92%) is achieved with IGOSTs including high crystalline P3HT film. The study provides fundamental information about the effects of polymer microstructure on synaptic plasticity of IGOSTs, which may be applicable in neuromorphic electronics.

Intrinsically stretchable organic light‐emitting diodes (ISOLEDs) are becoming essential components of wearable electronics. However, the efficiencies of ISOLEDs have been highly inferior compared with their rigid counterparts, which is due to the lack of ideal stretchable electrode materials that can overcome the poor charge injection at 1D metallic nanowire/organic interfaces. Herein, highly efficient ISOLEDs that use graphene‐based 2D‐contact stretchable electrodes (TCSEs) that incorporate a graphene layer on top of embedded metallic nanowires are demonstrated. The graphene layer modifies the work function, promotes charge spreading, and impedes inward diffusion of oxygen and moisture. The work function (WF) of 3.57 eV is achieved by forming a strong interfacial dipole after deposition of a newly designed conjugated polyelectrolyte with crown ether and anionic sulfonate groups on TCSE; this is the lowest value ever reported among ISOLEDs, which overcomes the existing problem of very poor electron injection in ISOLEDs. Subsequent pressure‐controlled lamination yields a highly efficient fluorescent ISOLED with an unprecedently high current efficiency of 20.3 cd A−1, which even exceeds that of an otherwise‐identical rigid counterpart. Lastly, a 3 inch five‐by‐five passive matrix ISOLED is demonstrated using convex stretching. This work can provide a rational protocol for designing intrinsically stretchable high‐efficiency optoelectronic devices with favorable interfacial electronic structures.