Preparing two‐dimensional conjugated polymers (2DCPs) with desirable structures and semiconducting properties is promising but remains a great challenge. Presented here is a new 2DCP, named 2D polytriethyltriindole (2DPTTI), which is efficiently synthesized by a modified interfacial Suzuki reaction from 2,7,12‐tribromo‐5,10,15‐triethyltriindole (2‐BrTTI) and 1,4‐benzenediboronic acid dipinacol ester (BADE) precursors at room temperature. Wafer‐scale free‐standing 2DPTTI films with controllable thicknesses between 2.5 and 46.0 nm were obtained by adjusting the experimental conditions. The resulting 2DPTTI films, used as an active layer in organic field effect transistors (OFETs), exhibited typical p‐type semiconducting properties and superior UV optoelectronic performance with a photosensitivity of 3.7×103 and responsivity of 1.4×103 A W−1, as well as a light‐blue fluorescence character. This report provides a general approach for constructing various semiconducting 2DCPs, by an interfacial Suzuki reaction, towards multifunctional organic electronics.

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A comprehensive summary and deep insights into the synthesis, characterization and multi-functional device applications of n-type and ambipolar organic semiconductors are provided in this study.

Electrically conductive coordination polymers (generally known as metal− organic frameworks, MOFs) are a class of crystalline hybrid materials produced by the reasonable self-assembly of metal nodes and organic linkers. The unique and intriguing combination of inorganic and organic components endows coordination polymers with superior optical and electrical properties, which have recently aroused much attention in several electronic and optoelectronic technological applications. However, there are many challenging obstacles and issues that need to be addressed in this burgeoning field. In this Perspective, we first provide a fundamental understanding about the electronic design strategies that provide better guidance for realizing high conductivities and good mobilities in coordination polymers. We then examine the current established synthetic approaches to construct high-quality working samples of electrically conductive coordination polymers for device integration. This is followed by a discussion of the current state-of-the-art progress toward the preliminary achievements in (opto)electronic devices spanning chemiresistive sensors, field-effect transistors, organic photovoltaics, photodetectors, etc. Finally, we conclude this Perspective with the existing hurdles and limitations in this area, along with the critical directions and opportunities for future research.

polarization over a wavelength range. The polarization-sensing ability offers them great advantages over typical photodetectors by enhancing image contrast and revealing hidden objects in various applications, such as target detection, remote sensing, security surveillance, as well as machine vision. [1,2] Generally, most polarization-sensitive photodetectors are realized on a complex system with the usage of optical sensors and photon-coupling components (polarizers or gratings). [1,3] However, such a strategy complicates device architecture, poses a challenge for their miniaturization on a chip, as well as limits their potential for integrating with flexible or wearable devices. Alternatively, exploiting "intrinsic linear dichroism" to realize polarization detection provides us a promising approach to circumvent above issues. [3][4][5][6][7][8][9][10][11][12] This strategy relies on the anisotropic optical properties, derived from the intrinsic anisotropic crystal structure, to achieve polarization sensitivity. In 2015, black phosphorus was successfully used to develop polarization-sensitive photodetectors by taking advantage of its unique in-plane anisotropic structure. [4] This work has inspired new interests of exploitingThe ability to detect light in photodetectors is central to practical optoelectronic applications, which has been demonstrated in inorganic semiconductor devices. However, so far, the study of polarization-sensitive organic photodetectors, which have unique applications in flexible and wearable electronics, has not received much attention. Herein, the construction of polarization-sensitive photodetectors based on the single crystals of a superior optoelectronic organic semiconductor, 2,6-diphenyl anthracene (DPA), is demonstrated. The systematic characterization of two-dimensionally grown DPA crystals with various techniques definitely show their strong anisotropy in molecular vibration, optical reflectance and optical absorption. In terms of polarization sensitivity, DPA-crystal based photodetectors exhibit a linear dichroic ratio up to ≈1.9. Theoretical calculations confirm that intrinsic linear dichroism, originated from the anisotropic in-plane crystal structure, is responsible for the polarization sensitivity of DPA crystals. This work opens up a new door for exploiting organic semiconductors for developing highly compact polarization photodetectors and providing new functionalities in novel flexible optical and optoelectronic applications. Dedicated to Prof. Daoben Zhu on the occasion of his 80th birthdayThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202105665.

This paper is NOT THE PUBLISHED VERSION; but the author's final, peer-reviewed manuscript. The published version may be accessed by following the link in th citation below.

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addressing probabilistic, and unstructured problems, thus is anticipated to solve the von Neumann bottleneck and become the mainstay of contemporary computing systems. [1,2] Synapses serve a crucial function in signal transmission in the biological neural system. [3] They transmit signals through neurotransmitters in a manner similar to that of field-effect transistors, where source-drain current changing in response to changes in gate voltage. In addition, organic materials are solutionprocessable, [4][5][6][7] thus simulating the functions of biological synapses by organic field-effect transistors has received intensive attention. [8,9] Most recently, higher performance requirements for devices are put forward to support practical applications, including fast switching speed, low energy consumption, low operating voltage, and strong compatibility with flexible substrate. Traditional planar field effect transistors struggle to accomplish these functions. Conversely, vertical organic field-effect transistors (VOFETs) have a more stable sourcedrain current and a changeable channel length that depends Organic field-effect transistors with parallel transmission and learning functions are of interest in the development of brain-inspired neuromorphic computing. However, the poor performance and high power consumption are the two main issues limiting their practical applications. Herein, an ultralowpower vertical transistor is demonstrated based on transition-metal carbides/ nitrides (MXene) and organic single crystal. The transistor exhibits a high J ON of 16.6 mA cm −2 and a high J ON /J OFF ratio of 9.12 × 10 5 under an ultralow working voltage of −1 mV. Furthermore, it can successfully simulate the functions of biological synapse under electrical modulation along with consuming only 8.7 aJ of power per spike. It also permits multilevel information decoding modes with a significant gap between the readable time of professionals and nonprofessionals, producing a high signal-to-noise ratio up to 114.15 dB. This work encourages the use of vertical transistors and organic single crystal in decoding information and advances the development of low-power neuromorphic systems.