Flexible electronics have attracted considerable attention recently given their potential to revolutionize human lives. High-performance organic crystalline materials (OCMs) are considered strong candidates for next-generation flexible electronics such as displays, image sensors, and artificial skin. They not only have great advantages in terms of flexibility, molecular diversity, low-cost, solution processability, and inherent compatibility with flexible substrates, but also show less grain boundaries with minimal defects, ensuring excellent and uniform electronic characteristics. Meanwhile, OCMs also serve as a powerful tool to probe the intrinsic electronic and mechanical properties of organics and reveal the flexible device physics for further guidance for flexible materials and device design. While the past decades have witnessed huge advances in OCM-based flexible electronics, this review is intended to provide a timely overview of this fascinating field. First, the crystal packing, charge transport, and assembly protocols of OCMs are introduced. State-of-the-art construction strategies for aligned/patterned OCM on/into flexible substrates are then discussed in detail. Following this, advanced OCM-based flexible devices and their potential applications are highlighted. Finally, future directions and opportunities for this field are proposed, in the hope of providing guidance for future research.

Organic crystalline materials in flexible electronics

Contact Resistance in Organic Field‐Effect Transistors: Conquering the Barrier

The field of organic electronics has been prolific in the last couple of years, leading to the design and synthesis of several molecular semiconductors presenting a mobility in excess of 10 cm2 V-1 s-1 . However, it is also started to recently falter, as a result of doubtful mobility extractions and reduced industrial interest. This critical review addresses the community of chemists and materials scientists to share with it a critical analysis of the best performing molecular semiconductors and of the inherent charge transport physics that takes place in them. The goal is to inspire chemists and materials scientists and to give them hope that the field of molecular semiconductors for logic operations is not engaged into a dead end. To the contrary, it offers plenty of research opportunities in materials chemistry.

https://onlinelibrary.wiley.com/doi/epdf/10.1002/adma.201905909

Molecular Semiconductors for Logic Operations: Dead-End or Bright Future?

The sensitivity of conventional thin-film OFET-based sensors is limited by the diffusion of analytes through bulk films and remains the central challenge in sensing technology. Now, for the first time, an ultrasensitive (sub-ppb level) sensor is reported that exploits n-type monolayer molecular crystals (MMCs) with porous two-dimensional structures. Thanks to monolayer crystal structure of NDI3HU-DTYM2 (NDI) and controlled formation of porous structure, a world-record detection limit of NH3 (0.1 ppb) was achieved. Moreover, the MMC-OFETs also enabled direct detection of solid analytes of biological amine derivatives, such as dopamine at an extremely low concentration of 500 ppb. The remarkably improved sensing performances of MMC-OFETs opens up the possibility of engineering OFETs for ultrasensitive (bio)chemical sensing.

https://www.onlinelibrary.wiley.com/doi/epdf/10.1002/anie.201916397

Monolayer Two-dimensional Molecular Crystals for an Ultrasensitive OFET-based Chemical Sensor.

The unique properties of hybrid heterostructures have motivated the integration of two or more different types of nanomaterials into a single optoelectronic device structure. Despite the promising features of organic semiconductors, such as their acceptable optoelectronic properties, availability of low-cost processes for their fabrication, and flexibility, further optimization of both material properties and device performances remains to be achieved. With the emergence of atomically thin 2D materials, they have been integrated with conventional organic semiconductors to form multidimensional heterostructures that overcome the present limitations and provide further opportunities in the field of optoelectronics. Herein, a comprehensive review of emerging 2D-organic heterostructures-from their synthesis and fabrication to their state-of-the-art optoelectronic applications-is presented. Future challenges and opportunities associated with these heterostructures are highlighted.

2D-Organic Hybrid Heterostructures for Optoelectronic Applications.

Organic thin-film transistors (OTFTs) with high mobility and low contact resistance have been actively pursued as building blocks for low-cost organic electronics. In conventional solution-processed or vacuum-deposited OTFTs, due to interfacial defects and traps, the organic film has to reach a certain thickness for efficient charge transport. Using an ultimate monolayer of 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) molecules as an OTFT channel, we demonstrate remarkable electrical characteristics, including intrinsic hole mobility over 30 cm2/Vs, Ohmic contact with 100 Ω · cm resistance, and band-like transport down to 150 K. Compared to conventional OTFTs, the main advantage of a monolayer channel is the direct, nondisruptive contact between the charge transport layer and metal leads, a feature that is vital for achieving low contact resistance and current saturation voltage. On the other hand, bilayer and thicker C8-BTBT OTFTs exhibit strong Schottky contact and much higher contact resistance but can be improved by inserting a doped graphene buffer layer. Our results suggest that highly crystalline molecular monolayers are promising form factors to build high-performance OTFTs and investigate device physics. They also allow us to precisely model how the molecular packing changes the transport and contact properties.

Tu Lan

Papers

Ultrahigh mobility and efficient charge injection in monolayer organic thin-film transistors on boron nitride