Aggregation-induced emission (AIE) describes a photophysical phenomenon in which molecular aggregates exhibit stronger emission than the single molecules. Over the course of the last 20 years, AIE research has made great strides in material development, mechanistic study and high-tech applications. The achievements of AIE research demonstrate that molecular aggregates show many properties and functions that are absent in molecular species. In this review, we summarize the advances in the field of AIE and its related areas. We specifically focus on the new properties of materials attained by molecular aggregates beyond the microscopic molecular level. We hope this review will inspire more research into molecular ensembles at and beyond the meso level and lead to the significant progress in material and biological science.

Aggregation-Induced Emission: New Vistas at the Aggregate Level

Next-generation wearable electronics will need to be mechanically flexible and stretchable such that they can be conformally attached onto the human body. Photodetectors that are available in today's market are based on rigid inorganic crystalline materials and they have limited mechanical flexibility. In contrast, photodetectors based on organic polymers and molecules have emerged as promising alternatives due to their inherent mechanical softness, ease of processing, tunable optoelectronic properties, good light sensing performance, and biocompatibility. Here, the recent advances of organic photodetectors in terms of both optoelectronic and mechanical properties are outlined and discussed, and their application in wearable electronics including health monitoring sensors, artificial vision, and self-powering integrated devices are highlighted.

Organic Photodetectors for Next-Generation Wearable Electronics.

Sunlight-driven water splitting to produce hydrogen fuel has stimulated intensive scientific interest, as this technology has the potential to revolutionize fossil fuel-based energy systems in modern society. The oxygen evolution reaction (OER) determines the performance of overall water splitting owing to its sluggish kinetics with multielectron transfer processing. Polymeric photocatalysts have recently been developed for the OER, and substantial progress has been realized in this emerging research field. In this Review, the focus is on the photocatalytic technologies and materials of polymeric photocatalysts for the OER. Two practical systems, namely, particle suspension systems and film-based photoelectrochemical systems, form two main sections. The concept is reviewed in terms of thermodynamics and kinetics, and polymeric photocatalysts are discussed based on three key characteristics, namely, light absorption, charge separation and transfer, and surface oxidation reactions. A satisfactory OER performance by polymeric photocatalysts will eventually offer a platform to achieve overall water splitting and other advanced applications in a cost-effective, sustainable, and renewable manner using solar energy.

Semiconducting Polymers for Oxygen Evolution Reaction under Light Illumination.

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Organic photodetectors based on supramolecular nanostructures

A luminescent cocrystal system is reported to undergo crystal-to-crystal phase transformation from yellow-emitting polymorph I to green-emitting polymorph II, triggered by THF fuming or heating, and the green emission can recover to the initial yellow emission by grinding. The established spectroscopic and crystallographic analyses demonstrate that the phase transition occurred and benefits from the combined effect of similar molecular arrange sequence and unique alteration of intermolecular interactions from halogen/hydrogen bonds in I to π-π stacking in II. Furthermore, I and II exhibit red-shift emission under hydrostatic pressure. The emission of I and II shows a red-shift and recovers towards the initial emission upon acid-base fuming. This is a rare example of reversible luminescent switching of cocrystal based upon crystal-to-crystal phase transition, and provides an alternative strategy to develop multi-stimuli responsive materials.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/anie.202008974

Reversible Luminescent Switching in an Organic Cocrystal: Multi-Stimuli-Induced Crystal-to-Crystal Phase Transformation

Construction of high-performance organic light-emitting transistors (OLETs) remains challenging due to the limited desired organic semiconductor materials. Here, two superior high mobility emissive organic semiconductors, 2,6-diphenylanthracene (DPA) and 2,6-di(2-naphthyl) anthracene (dNaAnt), are introduced into the construction of OLETs. By optimizing the device geometry for balanced ambipolar efficient charge transport and using high-quality DPA and dNaAnt single crystals as active layers, high-efficiency single-component OLETs are successfully fabricated, with the demonstration of strong and spatially controlled light emission within both p- and n- conducting channels and output of high external quantum efficiency (EQE). The obtained EQE values in current devices are approaching 1.61% for DPA-OLETs and 1.75% for dNaAnt-based OLETs, respectively, which are the highest EQE values for single-component OLETs in the common device configuration reported so far. Moreover, high brightnesses of 1210 and 3180 cd m-2 with current densities up to 1.3 and 8.4 kA cm-2 are also achieved for DPA- and dNaAnt-based OLETs, respectively. These results demonstrate the great potential applications of high mobility emissive organic semiconductors for next-generation rapid development of high-performance single-component OLETs and their related organic integrated electro-optical devices.

High-Efficiency Single-Component Organic Light-Emitting Transistors.

Here, we design and synthesize an organic laser molecule, 2,7-diphenyl-9H-fluorene (LD-1), which has state-of-the-art integrated optoelectronic properties with a high mobility of 0.25 cm2 V-1 s-1, a high photoluminescence quantum yield of 60.3%, and superior deep-blue laser characteristics (low threshold of Pth = 71 μJ cm-2 and Pth = 53 μJ cm-2 and high quality factor (Q) of ∼3100 and ∼2700 at emission peaks of 390 and 410 nm, respectively). Organic light-emitting transistors based on LD-1 are for the first time demonstrated with obvious electroluminescent emission and gate tunable features. This work opens the door for a new class of organic semiconductor laser molecules and is critical for deep-blue optical and laser applications.

Organic Laser Molecule with High Mobility, High Photoluminescence Quantum Yield, and Deep-Blue Lasing Characteristics

Organic light-emitting transistors (OLETs) are possibly the smallest integrated optoelectronic devices that combine the switching and amplification mechanisms of organic field-effect transistors (OFETs) and the electroluminescent characteristic of organic light-emitting diodes (OLEDs). Such a unique architecture of OLETs makes them ideal for developing the next-generation display technology and electrically pumped lasers for miniaturized photonic devices and circuits. However, the development of OLETs has been slow. Recently, some exciting progress has been made with breakthroughs in high mobility emissive organic semiconductors, construction of high-performance OLETs, and fabrication of novel multifunctional OLETs. This recent slew of advances may represent the advent of a new development stage of OLETs and their related devices and circuits. In this paper, a detailed review of these fantastic advances is presented, with a special focus on the key points for developing high-performance OLETs. Finally, a brief conclusion is provided with a discussion on the challenges and future perspectives in this field.

Organic Light-Emitting Transistors Entering a New Development Stage

Vertical Organic Field-Effect Transistors

Herein, two kinds of vertical organic optoelectronic devices, vertical organic field-effect transistors (VOFETs) and light-emitting transistors (VOLETs), were constructed based on amorphous organic semiconductors of N,N'-di(1-naphthyl)-N,N'-diphenyl-(1,1'-biphenyl)-4,4'-diamine (NPB) as hole injecting and transport layers and tris(8-hydroxy-quinolinato) aluminum (Alq3) as the emitting layer. High device performances with a large on/off ratio of ∼6 × 103, current density of ∼40 mA cm-2, and fast response of ∼5 ms at a frequency of 20 Hz and a brightness of 126 cd m-2 were demonstrated for these two vertical devices with good device stability and repeatability. These results suggest the potential applications of amorphous organic semiconductors with good film-forming characteristics and easy device fabrication ability in vertical optoelectronic circuits.

Haikuo Gao

Papers

High-Efficiency Single-Component Organic Light-Emitting Transistors.

Organic Laser Molecule with High Mobility, High Photoluminescence Quantum Yield, and Deep-Blue Lasing Characteristics

Organic Light-Emitting Transistors Entering a New Development Stage

Vertical Organic Field-Effect Transistors

High-performance amorphous organic semiconductor-based vertical field-effect transistors and light-emitting transistors