Covalent Bond Torsion-Enabled Unique Crystal-Phase Transformation of an Organic Semiconductor for Multicolor Light-Emitting Transistors.

High-mobility and color-tunable highly emissive organic semiconductors (OSCs) are highly promising for various optoelectronic device applications and novel structure-property relationship investigations. However, such OSCs have never been reported because of the great trade-off between mobility, emission color, and emission efficiency. Here, we report a novel strategy of molecular conformation-induced unique crystalline polymorphism to realize the high mobility and color-tunable high emission in a novel OSC, 2,7-di(anthracen-2-yl) naphthalene (2,7-DAN). Interestingly, 2,7-DAN has unique crystalline polymorphism, which has an almost identical packing motif but slightly different molecular conformation enabled by the small bond rotation angle variation between anthracene and naphthalene units. More remarkably, the subtle covalent bond rotation angle change leads to a big change in color emission (from blue to green) but does not significantly modify the mobility and emission efficiency. The carrier mobility of 2,7-DAN crystals can reach up to a reliable 17 cm2 V-1 s-1, which is rare for the reported high-mobility OSCs. Based on the unique phenomenon, high-performance light-emitting transistors with blue to green emission are simultaneously demonstrated in an OSC crystal. These results open a new way for designing emerging multifunctional organic semiconductors toward next-generation advanced molecular (atomic)-scale optoelectronics devices.

Highly-Polarized Solar-Blind Ultraviolet Organic Photodetectors.

Developing high-performance polarization-sensitive ultraviolet photodetectors is crucial for their application in military remote sensing, detection, bio-inspired navigation, and machine vision. However, the significant absorption in the visible light range severely limits the application of polarization-sensitive ultraviolet photodetectors, such as high-quality anti-interference imaging. Here, based on a wide-bandgap organic semiconductor single crystal (trans-1,2-bis(5-phenyldithieno[2,3-b:3',2'-d]thiophen-2-yl)ethene, BPTTE), high-performance polarization-sensitive solar-blind ultraviolet photodetectors with a dichroic ratio close to 4.26 are demonstrated. The strong anisotropy of 2D grown BPTTE single crystals in molecular vibration and optical absorption is characterized by various techniques. Under voltage modulation, stable and efficient detection of polarized light is demonstrated, attributed to the intrinsic anisotropy of transition dipole moment in the bc crystal plane, rather than other factors. Finally, high-contrast polarimetric imaging and anti-interference imaging are successfully demonstrated based on BPTTE single crystal photodetectors, highlighting the potential of organic semiconductors for polarization-sensitive solar-blind ultraviolet photodetectors.

High-Efficiency Area-Emissive White Organic Light-Emitting Transistor for Full-Color Display.

The construction of high-performance white organic light-emitting transistor (OLET) with uniform area emission is crucial for smart display technologies but remains greatly challenging. Herein, high-efficiency uniform area-emissive OLETs based on a unique lateral-integrated device configuration which incorporates efficient energy transfer of phosphorescent and fluorescent guests, enabling color-tunable and white emission, are demonstrated. Through precisely regulating the energy transfer between host and guests, high external quantum efficiency of 13.9% for white-emission OLETs is achieved due to the improved high exciton utilization and light outcoupling efficiency which is the highest value reported so far for OLETs and prevents exciton-charge annihilation and electrode photon losses. Moreover, good loop stability is also achieved, along with effective gate tunability and ultralow driving voltage of below 5 V. Finally, a 4 × 6 white-emission OLET array for full-color display is demonstrated for the first time, suggesting its great potential applications for advanced display technologies.

Dibenzothiophene Sulfone-Based Ambipolar-Transporting Blue-Emissive Organic Semiconductors Towards Simple-Structured Organic Light-Emitting Transistors.

The development of blue-emissive ambipolar organic semiconductor is an arduous target due to the large energy gap, but is an indispensable part for electroluminescent device, especially for the transformative display technology of simple-structured organic light-emitting transistor (SS-OLET). Herein, we designed and synthesized two new dibenzothiophene sulfone-based high mobility blue-emissive organic semiconductors (DNaDBSOs), which demonstrate superior optical property with solid-state photoluminescent quantum yield of 46-67 % and typical ambipolar-transporting properties in SS-OLETs with symmetric gold electrodes. Comprehensive experimental and theoretical characterizations reveal the natural of ambipolar property for such blue-emissive DNaDBSOs-based materials is ascribed to a synergistic effect on lowering LUMO level and reduced electron injection barrier induced by the interfacial dipoles effect on gold electrodes due to the incorporation of appropriate DBSO unit. Finally, efficient electroluminescence properties with high-quality blue emission (CIE (0.179, 0.119)) and a narrow full-width at half-maximum of 48 nm are achieved for DNaDBSO-based SS-OLET, showing good spatial control of the recombination zone in conducting channel. This work provides a new avenue for designing ambipolar emissive organic semiconductors by incorporating the synergistic effect of energy level regulation and molecular-metal interaction, which would advance the development of superior optoelectronic materials and their high-density integrated optoelectronic devices and circuits.

Organic Polarized Light-Emitting Transistors.

Electrically driven polarized light-emitting sources are central to various applications including quantum computers, optical communication, and 3D displays, but serious challenges remain due to the inevitable incorporation of complex optical elements in conventional devices. Here, organic polarized light-emitting transistors (OPLETs), a kind of novel device that integrates the functions of organic field-effect transistors, organic light-emitting diodes, and polarizers into one unique device, are demonstrated with a degree of polarization (DOP) as high as 0.97, which is comparable to completely linearly polarized light (DOP = 1). Under the modulation of gate voltage, robust and efficient polarization emission is proven, ascribed to the intrinsic in-plane anisotropy of the molecular transition dipole moment in organic semiconductors and the open-ended feature of OPLETs instead of other factors. As a result, high-contrast optical imaging and anti-counterfeiting security are successfully demonstrated based on OPLETs, establishing a new direction for photonic and electronic integration toward on-chip miniaturized optoelectronic applications.

High-Performance Ambipolar and n-Type Emissive Semiconductors Based on Perfluorophenyl-Substituted Perylene and Anthracene.

Emissive organic semiconductors are highly demanding for organic light-emitting transistors (OLETs) and electrically pumped organic lasers (EPOLs). However, it remains a great challenge to obtain organic semiconductors with high carrier mobility and high photoluminescence quantum yield simultaneously. Here, a new design strategy is reported for highly emissive ambipolar and even n-type semiconductors by introducing perfluorophenyl groups into polycyclic aromatic hydrocarbons such as perylene and anthracene. The results reveal that 3,9-diperfluorophenyl perylene (5FDPP) exhibits the ambipolar semiconducting property with hole and electron mobilities up to 0.12 and 1.89 cm2 V-1 s-1 , and a photoluminescence quantum yield of 55%. One of the crystal forms of 5FDPA exhibits blue emission with an emission quantum yield of 52% and simultaneously shows the n-type semiconducting property with an electron mobility up to 2.65 cm2 V-1 s-1 , which is the highest value among the reported organic emissive n-type semiconductors. Furthermore, crystals of 5FDPP are utilized to fabricate OLETs by using Ag as source-drain electrodes. The electroluminescence is detected in the transporting channels with an external quantum efficiency (EQE) of up to 2.2%, and the current density is up to 145 kA cm-2 , which are among the highest values for single-component OLETs with symmetric electrodes.

Regulating Crystal Packing by Terminal tert-Butylation for Enhanced Solid-State Emission and Efficacious Charge Transport in an Anthracene-Based Molecular Crystal.

Organic semiconductors with combinative high carrier mobility and efficient solid-state emission are full of challenges but urgently pursued for developing new emerging optoelectronics. Herein, by delicately regulating the crystal packing of an anthracene-based molecular crystal via terminal tert-butylation, we developed a superior high mobility emissive molecule, 2,6-di(6-tert-butylnaphthyl)anthracene (TBU-DNA). The unique "slipped herringbone" packing motif of TBU-DNA enables its appropriate exciton-exciton coupling and electron-phonon coupling, thus resulting in remarkably high solid-state emission (photoluminescence quantum yield, ΦF ≈74.9 %) and efficacious charge transport (carrier mobility, µ=5.0 cm2 V-1 s-1 ). Furthermore, OLETs based on TBU-DNA show an external quantum efficiency (EQE) of 1.8 %, which is among the highest EQE values for single component OLETs reported till now. This work presents a crystal engineering strategy via exquisite molecular design to realize high mobility emissive organic semiconductors.

Molecular doped, color-tunable, high-mobility, emissive, organic semiconductors for light-emitting transistors.

Developing high-mobility emissive organic semiconductors with tunable colors is crucial for organic light-emitting transistors (OLETs), a pivotal component of integrated optoelectronic devices, but remains a great challenge. Here, we demonstrate a series of color-tunable, high-mobility, emissive, organic semiconductors via molecular doping with a high-mobility organic semiconductor, 2,6-diphenylanthracene, as the host. The well-matched molecular structures and sizes with efficient energy transfer between the host and guest enable the intrinsically high charge transport with tunable colors. High mobility with the highest value >2 cm2 V-1 s-1 and strong emission with photoluminescence quantum yield >15.8% are obtained for these molecular-doped organic semiconductors. Last, a large color gamut for constructed OLETs is up to 59% National Television System Committee standard, meanwhile with an extremely high current density approaching 326.4 kA cm-2, showing great potential for full-color smart display, organic electrically pumped lasers and other related logic circuitries.

Redistributed Current Density in Lateral Organic Light-Emitting Transistors Enabling Uniform Area Emission with Good Stability and Arbitrary Tunability.

Organic light-emitting transistors (OLETs), integrating the functions of an organic field-effect transistor (OFET) and organic light-emitting diode (OLED) in a single device, are promising for the next-generation display technology. However, the great challenge of achieving uniform area emission in OLETs with good stability and arbitrary tunability hinders their development in this field. Herein, an effective solution to obtain well-defined area emission in lateral OLETs by incorporating a charge-transport buffer (CTB) layer between the conducting channel and emitting layer is proposed. Comprehensive theoretical simulation and experimental results demonstrate redistributed potential beneath the drain electrode under the shielding effect of the CBT layer, resulting in a highly uniform current density. In this case, uniform recombination of balanced holes and electrons can be guaranteed, which is essential for the formation of area emission in the following OLETs. RGB OLETs with uniform area emission are constructed, which show good gate tunable ability (ON/OFF ratio 106 ), high loop stability (over 200 cycles) and high aperture ratio (over 80%) due to the arbitrary tunability of the device geometry. This work provides a new avenue for constructing area-emission lateral OLETs, which have great potential for display technology because of their good compatibility with conventional fabrication techniques.

Intrinsic Linear Dichroism of Organic Single Crystals toward High-Performance Polarization-Sensitive Photodetectors.

The 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.

Application of Triplet-Triplet Annihilation Upconversion in Organic Optoelectronic Devices: Advances and Perspectives.

Organic semiconductor materials have been widely used in various optoelectronic devices due to their rich optical and/or electrical properties, which are highly related to their excited states. Therefore, how to manage and utilize the excited states in organic semiconductors is essential for the realization of high-performance optoelectronic devices. Triplet-triplet annihilation (TTA) upconversion is a unique process of converting two non-emissive triplet excitons to one singlet exciton with higher energy. Efficient optical-to-electrical devices can be realized by harvesting sub-bandgap photons through TTA-based upconversion. In electrical-to-optical devices, triplets generated after the combination of electrons and holes also can be efficiently utilized via TTA, which resulted in a high internal conversion efficiency of 62.5%. Currently, many interesting explorations and significant advances have been demonstrated in these fields. In this review, a comprehensive summary of these intriguing advances on developing efficient TTA upconversion materials and their application in optoelectronic devices is systematically given along with some discussions. Finally, the key challenges and perspectives of TTA upconversion systems for further improvement for optoelectronic devices and other related research directions are provided. This review hopes to provide valuable guidelines for future related research and advancement in organic optoelectronics.

High Mobility Organic Lasing Semiconductor with Crystallization-Enhanced Emission for Light-Emitting Transistors.

The development of high mobility organic laser semiconductors with strong emission is of great scientific and technical importance, but challenging. Herein, we present a high mobility organic laser semiconductor, 2,7-diphenyl-9H-fluorene (LD-1) showing unique crystallization-enhanced emission guided by elaborately modulating its crystal growth process. The obtained one-dimensional nanowires of LD-1 show outstanding integrated properties including: high absolute photoluminescence quantum yield (PLQY) approaching 80 %, high charge carrier mobility of 0.08 cm2 V-1 s-1 , Fabry-Perot lasing characters with a low threshold of 86 µJ cm-2 and a high-quality factor of ≈2400. Furthermore, electrically induced emission was obtained from an individual LD-1 crystal nanowire-based light-emitting transistor due to the recombination of holes and electrons simultaneously injected into the nanowire, which provides a good platform for the study of electrically pumped organic lasers and other related ultrasmall integrated electrical-driven photonic devices.

Organic Light-Emitting Transistors Entering a New Development Stage.

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.

Electrically Conductive Coordination Polymers for Electronic and Optoelectronic Device Applications.

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.

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

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

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 UV-Sensitive Phototransistors Based on Distriphenylamineethynylpyrene Derivatives with Ultra-High Detectivity Approaching 1018.

Organic photodetectors with UV-sensitivity are of great potential for various optoelectronic applications. Integration of high charge carrier mobility, long exciton diffusion length as well as unique UV-sensitivity for active materials is crucial for construction of UV-sensitive devices with high performance, however, very few organic semiconductors can integrate these properties simultaneously. Herein, two novel organic semiconductors containing large steric hindrance triphenylamine groups, 1,6-distriphenylamineethynylpyrene (1,6-DTEP) and 2,7-distriphenylamineethynylpyrene (2,7-DTEP) are designed and synthesized. It demonstrates that the single crystals of both 1,6-DTEP and 2,7-DTEP exhibit superior integrated optoelectronic properties of high charge carrier mobility, unique UV absorption, high photoluminescence quantum yields as well as small exciton binding energies. Organic phototransistors constructed using 1,6-DTEP and 2,7-DTEP single crystals show ultrasensitive performance with ultra-high photoresponsivity of 2.86 × 106 and 1.04 × 105 A W-1 , detectivity (D*) of above 1.49 × 1018 and 5.28 × 1016 Jones under 370 nm light illumination, respectively. It indicates the great potential of 1,6-DTEP and 2,7-DTEP-based phototransistors for organic UV-photodetector applications and also provides a new design strategy to develop series of better performance UV photoelectric organic materials for related research in organic optoelectronics.

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

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.