Intrinsic Self-Trapped Excitons in Graphitic Carbon Nitride.

Graphitic carbon nitrides (g-C3N4) as low-cost, chemically stable, and ecofriendly layered semiconductors have attracted rapidly growing interest in optoelectronics and photocatalysis. However, the nature of photoexcited carriers in g-C3N4 is still controversial, and an independent charge-carrier picture based on the band theory is commonly adopted. Here, by performing transient spectroscopy studies, we show characteristics of self-trapped excitons (STEs) in g-C3N4 nanosheets including broad trapped exciton-induced absorption, picosecond exciton trapping without saturation at high photoexcitation density, and transient STE-induced stimulated emissions. These features, together with the ultrafast exciton trapping polarization memory, strongly suggest that STEs intrinsically define the nature of the photoexcited states in g-C3N4. These observations provide new insights into the fundamental photophysics of carbon nitrides, which may enlighten novel designs to boost energy conversion efficiency.

Correction: Atomically flat semiconductor nanoplatelets for light-emitting applications.

Correction for 'Atomically flat semiconductor nanoplatelets for light-emitting applications' by Bing Bai et al., Chem. Soc. Rev., 2023, 52, 318-360, https://doi.org/10.1039/D2CS00130F.

Atomically flat semiconductor nanoplatelets for light-emitting applications.

The last decade has witnessed extensive breakthroughs and significant progress in atomically flat two-dimensional (2D) semiconductor nanoplatelets (NPLs) in terms of synthesis, growth mechanisms, optical and electronic properties and practical applications. Such NPLs have electronic structures similar to those of quantum wells in which excitons are predominantly confined along the vertical direction, while electrons are free to move in the lateral directions, resulting in unique optical properties, such as extremely narrow emission line width, short photoluminescence (PL) lifetime, high gain coefficient, and giant oscillator strength transition (GOST). These unique optical properties make NPLs favorable for high color purity light-emitting applications, in particular in light-emitting diodes (LEDs), backlights for liquid crystal displays (LCDs) and lasers. This review article first introduces the intrinsic characteristics of 2D semiconductor NPLs with atomic flatness. Subsequently, the approaches and mechanisms for the controlled synthesis of atomically flat NPLs are summarized followed by an insight on recent progress in the mediation of core/shell, core/crown and core/crown@shell structures by selective epitaxial growth of passivation layers on different planes of NPLs. Moreover, an overview of the unique optical properties and the associated light-emitting applications is elaborated. Despite great progress in this research field, there are some issues relating to heavy metal elements such as Cd2+ in NPLs, and the ambiguous gain mechanisms of NPLs and others are the main obstacles that prevent NPLs from widespread applications. Therefore, a perspective is included at the end of this review article, in which the current challenges in this stimulating research field are discussed and possible solutions to tackle these challenges are proposed.

Observation of Phonon Cascades in Cu-Doped Colloidal Quantum Wells.

Electronic doping has endowed colloidal quantum wells (CQWs) with unique optical and electronic properties, holding great potential for future optoelectronic device concepts. Unfortunately, how photogenerated hot carriers interact with phonons in these doped CQWs still remains an open question. Here, through investigating the emission properties, we have observed an efficient phonon cascade process (i.e., up to 27 longitudinal optical phonon replicas are revealed in the broad Cu emission band at room temperature) and identified a giant Huang-Rhys factor (S ≈ 12.4, more than 1 order of magnitude larger than reported values of other inorganic semiconductor nanomaterials) in Cu-doped CQWs. We argue that such an ultrastrong electron-phonon coupling in Cu-doped CQWs is due to the dopant-induced lattice distortion and the dopant-enhanced density of states. These findings break the widely accepted consensus that electron-phonon coupling is typically weak in quantum-confined systems, which are crucial for optoelectronic applications of doped electronic nanomaterials.

Deep-Red-Emitting Colloidal Quantum Well Light-Emitting Diodes Enabled through a Complex Design of Core/Crown/Double Shell Heterostructure.

Extending the emission peak wavelength of quasi-2D colloidal quantum wells has been an important quest to fully exploit the potential of these materials, which has not been possible due to the complications arising from the partial dissolution and recrystallization during growth to date. Here, the synthetic pathway of (CdSe/CdS)@(1-4 CdS/CdZnS) (core/crown)@(colloidal atomic layer deposition shell/hot injection shell) hetero-nanoplatelets (NPLs) using multiple techniques, which together enable highly efficient emission beyond 700 nm in the deep-red region, is proposed and demonstrated. Given the challenges of using conventional hot injection procedure, a method that allows to obtain sufficiently thick and passivated NPLs as the seeds is developed. Consequently, through the final hot injection shell coating, thick NPLs with superior optical properties including a high photoluminescence quantum yield of 88% are achieved. These NPLs emitting at 701 nm exhibit a full-width-at-half-maximum of 26 nm, enabled by the successfully maintained quasi-2D shape and minimum defects of the resulting heterostructure. The deep-red light-emitting diode (LED) device fabricated with these NPLs has shown to yield a high external quantum efficiency of 6.8% at 701 nm, which is on par with other types of LEDs in this spectral range.

Achieving Solution-Processed Non-Doped Single-Emitting-Layer White Organic Light-Emitting Diodes through Adjusting Pyrene-Based Polyaromatic Hydrocarbon.

Single-emitting-layer white organic light-emitting diodes (SEL-WOLEDs) have developed rapidly in recent years due to the outstanding advantages of high efficiency, simple device structure, low cost, less phase separation, and stable emission color. Nevertheless, the relatively complicated host-dopant system is usually essential for most previous SEL-WOLEDs and the development of simple non-doped SEL-WOLEDs lags behind. Hence the straightforward synthesis of single-white-emitting molecules for non-doped SEL-WOLEDs still remains a great challengeable task. In this article, we designed and synthesized two new pyrene-based polyaromatic hydrocarbons (PAHs) and used them as emitting layer materials in the OLED devices. When the molecules change from the mono-fused one to bis-fused one, the emitting light changes from greenish to white color. Further study indicated that the bis-fused molecule PyD with more twisted and extended backbone packed in neat Cmca space group in single-crystal system compared with P21 /n for PyS, which may be favorable to form excimers in the solid state and broaden the emission spectrum in the OLEDs. As a result, a solution-processed non-doped single-white-emitting-molecule SEL-WOLED with high performance (e. g., a high color rendering index of 66) is reported. The findings will be beneficial not only to further development of simple WOLEDs, but also to other related organic optoelectronic technology.

An Electrochemical Sensor Based on Electropolymerization of ß-Cyclodextrin on Glassy Carbon Electrode for the Determination of Fenitrothion.

An electrochemical sensor enabled by electropolymerization (EP) of ß-cyclodextrin on glassy carbon electrode (ß-CDP/GCE) is built for the determination of fenitrothion (FNT). The effects of the EP cycles, pH value, and enrichment time on the electrochemical response of FNT were studied. With the optimum conditions, good linear relationships between the current of the reduction peak of the nitroso derivative of FNT and the concentration are obtained in the range of 10-150 and 150-4000 ng/mL, with a detection limit of 6 ng/mL (S/N = 3). ß-CDP/GCE also exhibits a satisfactory applicability in cabbage and tap water, with recovery values between 98.43% and 112%. These outstanding results suggest that ß-CDP/GCE could be a new effective alternative for the determination of FNT in real samples.

Light-Emitting Diodes with Cu-Doped Colloidal Quantum Wells: From Ultrapure Green, Tunable Dual-Emission to White Light.

Copper-doped colloidal quantum wells (Cu-CQWs) are considered a new class of optoelectronic materials. To date, the electroluminescence (EL) property of Cu-CQWs has not been revealed. Additionally, it is desirable to achieve ultrapure green, tunable dual-emission and white light to satisfy the various requirement of display and lighting applications. Herein, light-emitting diodes (LEDs) based on colloidal Cu-CQWs are demonstrated. For the 0% Cu-doped concentration, the LED exhibits Commission Internationale de L'Eclairage 1931 coordinates of (0.103, 0.797) with a narrow EL full-wavelength at half-maximum of 12 nm. For the 0.5% Cu-doped concentration, a dual-emission LED is realized. Remarkably, the dual emission can be tuned by manipulating the device engineering. Furthermore, at a high doping concentration of 2.4%, a white LED based on CQWs is developed. With the management of doping concentrations, the color tuning (green, dual-emission to white) is shown. The findings not only show that LEDs with CQWs can exhibit polychromatic emission but also unlock a new direction to develop LEDs by exploiting 2D impurity-doped CQWs that can be further extended to the application of other impurities (e.g., Mn, Ag).

Doping-Free White Organic Light-Emitting Diodes.

Doping-free white organic light-emitting diodes (WOLEDs) have great potential to the next-generation solid-state lighting and displays due to the excellent properties, such as high efficiency, bright luminance, low power consumption, simplified structure and low cost. In this account, our recent developments on doping-free WOLEDs have been summarized. Firstly, fundamental concepts of doping-free WOLEDs have been described. Then, the effective strategies to develop doping-free WOLEDs have been presented. Particularly, the manipulation of charges and excitons distribution in different kinds of doping-free WOLEDs have been highlighted, including doping-free fluorescent/phosphorescent hybrid WOLEDs, doping-free thermally activated delayed fluorescent WOLEDs and doping-free phosphorescent WOLEDs. In the end, an outlook for the future development of doping-free WOLEDs have been clarified.

Recent Developments in Tandem White Organic Light-Emitting Diodes.

Tandem white organic light-emitting diodes (WOLEDs) are promising for the lighting and displays field since their current efficiency, external quantum efficiency and lifetime can be strikingly enhanced compared with single-unit devices. In this invited review, we have firstly described fundamental concepts of tandem device architectures and their use in WOLEDs. Then, we have summarized the state-of-the-art strategies to achieve high-performance tandem WOLEDs in recent years. Specifically, we have highlighted the developments in the four types of tandem WOLEDs (i.e., tandem fluorescent WOLEDs, tandem phosphorescent WOLEDs, tandem thermally activated delayed fluorescent WOLEDs, and tandem hybrid WOLEDs). Furthermore, we have introduced doping-free tandem WOLEDs. In the end, we have given an outlook for the future development of tandem WOLEDs.

Room-Temperature Fabricated Thin-Film Transistors Based on Compounds with Lanthanum and Main Family Element Boron.

For the first time, compounds with lanthanum from the main family element Boron (LaBx) were investigated as an active layer for thin-film transistors (TFTs). Detailed studies showed that the room-temperature fabricated LaBx thin film was in the crystalline state with a relatively narrow optical band gap of 2.28 eV. The atom ration of La/B was related to the working pressure during the sputtering process and the atom ration of La/B increased with the increase of the working pressure, which will result in the freer electrons in the LaBx thin film. LaBx-TFT without any intentionally annealing steps exhibited a saturation mobility of 0.44 cm²·V−1·s−1, which is a subthreshold swing (SS) of 0.26 V/decade and a Ion/Ioff ratio larger than 104. The room-temperature process is attractive for its compatibility with almost all kinds of flexible substrates and the LaBx semiconductor may be a new choice for the channel materials in TFTs.

Approaches to Enhance the Stability of Colloidal Quantum Well Light- Emitting Diodes.

Colloidal quantum well light-emitting diodes (CQW-LEDs) show great potential for applications in displays and lighting due to their advantages, such as high color purity, spectral tunability and compatibility with flexible electronics. So far, attention has been mainly devoted to pursuing device efficiencies rather than achieving device stability, leading to the fact that the lifetime of CQW-LEDs is far from the demand for practical applications. In this perspective, various approaches to enhance the stability of CQW-LEDs have been discussed, including the synthesis of stable CQW materials, the selection of stable transport layers, the improvement of charge balance, and the introduction of advanced encapsulation techniques.

An Artificial Neural Network Based on Oxide Synaptic Transistor for Accurate and Robust Image Recognition.

Synaptic transistors with low-temperature, solution-processed dielectric films have demonstrated programmable conductance, and therefore potential applications in hardware artificial neural networks for recognizing noisy images. Here, we engineered AlOx/InOx synaptic transistors via a solution process to instantiate neural networks. The transistors show long-term potentiation under appropriate gate voltage pulses. The artificial neural network, consisting of one input layer and one output layer, was constructed using 9 × 3 synaptic transistors. By programming the calculated weight, the hardware network can recognize 3 × 3 pixel images of characters z, v and n with a high accuracy of 85%, even with 40% noise. This work demonstrates that metal-oxide transistors, which exhibit significant long-term potentiation of conductance, can be used for the accurate recognition of noisy images.

Understanding Quasi-Static and Dynamic Characteristics of Organic Ferroelectric Field Effect Transistors.

Leveraging poly(vinylidene fluoride-trifluoroethylene) [(PVDF-TrFE)] as the dielectric, we fabricated organic ferroelectric field-effect transistors (OFe-FETs). These devices demonstrate quasi-static transfer characteristics that include a hysteresis window alongside transient phenomena that bear resemblance to synaptic plasticity-encapsulating excitatory postsynaptic current (EPSC) as well as both short-term and long-term potentiation (STP/LTP). We also explore and elucidate other aspects such as the subthreshold swing and the hysteresis window under dynamic state by varying the pace of voltage sweeps. In addition, we developed an analytical model that describes the electrical properties of OFe-FETs, which melds an empirical formula for ferroelectric polarization with a compact model. This model agrees well with the experimental data concerning quasi-static transfer characteristics, potentially serving as a quantitative tool to improve the understanding and design of OFe-FETs.

Manipulation of Charge Dynamics for Efficient and Bright Blue Perovskite Light-Emitting Diodes with Chiral Ligands.

Perovskite light-emitting diodes (PeLEDs) emerge as a promising class of optoelectronic devices for next-generation displays and lighting technology. However, the performance of blue PeLEDs lags far behind that of their green and red counterparts, including the unachieved trade-off between high efficiency and high luminance, severe efficiency roll-off, and unsatisfactory power efficiency. Here, a multi-functional chiral ligand of L-phenylalanine methyl ester hydrochloride is strategically introduced into quasi-2D perovskites, which can effectively passivate defects, modulate the phase distribution, improve photoluminescence quantum yield, guarantee high-quality film morphology, and enhance charge transport. Furthermore, ladder-like hole transport layers are established, boosting charge injection and balance. The resultant sky-blue PeLEDs (the photoluminescence peak is 493 nm and the electroluminescence peak is 497 nm) exhibit an external quantum efficiency of 12.43% at 1000 cd m-2 and a record power efficiency of 18.42 lm W-1 , rendering that the performance is among the best blue PeLEDs.

High-Performance Solar-Blind UV Phototransistors Based on ZnO/Ga2O3 Heterojunction Channels.

High-performance phototransistor-based solar-blind (200-280 nm) ultraviolet (UV) photodetectors (PDs) are constructed with a low-cost thin-film ZnO/Ga2O3 heterojunction. The optimized PD shows high spectral selectivity (R254/R365 > 1 × 103) with a photo-to-dark current ratio of ∼104, a responsivity of 113 mA/W, a detectivity of 1.25 × 1012 Jones, and a response speed of 41 ms under 254 nm UV light irradiation. It is found that the gate electrode of a three-terminal phototransistor can amplify the responsivity and increase the photo-to-dark current ratio because of the different densities of field-induced electrons at different gate biases. In addition, the built-in electric field at the ZnO/Ga2O3 heterojunction interface can control the distribution of the photoinduced electrons and the total conductivity of the heterojunction, which can further enhance device performance. Together with the simple fabrication process, the achieved results suggest that the three-terminal ZnO/Ga2O3 heterojunction phototransistor is a promising candidate for highly sensitive solar-blind PDs.

High External Quantum Efficiency Light-Emitting Diodes Enabled by Advanced Heterostructures of Type-II Nanoplatelets.

Colloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts. Unlike traditional type-II NPLs such as CdSe/CdTe, CdTe/CdSe, and CdSe/CdSexTe1-x core/crown heterostructures, here the proposed advanced heterostructure reaps the benefits of having two type-II transition channels, resulting in a high quantum yield (QY) of 83% and a long fluorescence lifetime of 73.3 ns. These type-II transitions were confirmed experimentally by optical measurements and theoretically using electron and hole wave function modeling. Computational study shows that the multi-crowned NPLs provide a better-distributed hole wave function along the CdTe crown, while the electron wave function is delocalized in the CdSe core and CdSe crown layers. As a proof-of-concept demonstration, NPL-LEDs based on these multi-crowned NPLs were designed and fabricated with a record high external quantum efficiency (EQE) of 7.83% among type-II NPL-LEDs. These findings are expected to induce advanced designs of NPL heterostructures to reach a fascinating level of performance, especially in LEDs and lasers.

Understanding the Structure and Energy Transfer Process of Undoped Ultrathin Emitting Nanolayers Within Interface Exciplexes.

Organic light-emitting diodes (OLEDs) have great potential for display, lighting, and near-infrared (NIR) applications due to their outstanding advantages such as high efficiency, low power consumption, and flexibility. Recently, it has been found that the ultrathin emitting nanolayer technology plays a key role in OLEDs with simplified structures through the undoped fabricated process, and exciplex-forming hosts can enhance the efficiency and stability of OLEDs. However, the elementary structure and mechanism of the energy transfer process of ultrathin emitting nanolayers within interface exciplexes are still unclear. Therefore, it is imminently needed to explore the origin of ultrathin emitting nanolayers and their energy process within exciplexes. Herein, the mechanism of films growing to set ultrathin emitting nanolayers (<1 nm) and their energy transfer process within interface exciplexes are reviewed and researched. The UEML phosphorescence dye plays a key role in determining the lifetime of excitons between exciplex and non-exciplex interfaces. The exciplex between TCTA and Bphen has longer lifetime decay than the non-exciplex between TCTA and TAPC, facilitating exciton harvesting. The findings will be beneficial not only to the further development of OLEDs but also to other related organic optoelectronic technologies.

High-Performance Deep Red Colloidal Quantum Well Light-Emitting Diodes Enabled by the Understanding of Charge Dynamics.

Colloidal quantum wells (CQWs) have emerged as a promising family of two-dimensional (2D) optoelectronic materials with outstanding properties, including ultranarrow luminescence emission, nearly unity quantum yield, and large extinction coefficient. However, the performance of CQWs-based light-emitting diodes (CQW-LEDs) is far from satisfactory, particularly for deep red emissions (≥660 nm). Herein, high efficiency, ultra-low-efficiency roll-off, high luminance, and extremely saturated deep red CQW-LEDs are reported. A key feature for the high performance is the understanding of charge dynamics achieved by introducing an efficient electron transport layer, ZnMgO, which enables balanced charge injection, reduced nonradiative channels, and smooth films. The CQW-LEDs based on (CdSe/CdS)@(CdS/CdZnS) ((core/crown)@(colloidal atomic layer deposition shell/hot injection shell)) show an external quantum efficiency of 9.89%, which is a record value for 2D nanocrystal LEDs with deep red emissions. The device also exhibits an ultra-low-efficiency roll-off and a high luminance of 3853 cd m-2. Additionally, an exceptional color purity with the CIE coordinates of (0.719, 0.278) is obtained, indicating that the color gamut covers 102% of the International Telecommunication Union Recommendation BT 2020 (Rec. 2020) standard in the CIE 1931 color space, which is the best for CQW-LEDs. Furthermore, an active-matrix CQW-LED pixel circuit is demonstrated. The findings imply that the understanding of charge dynamics not only enables high-performance CQW-LEDs and can be further applied to other kinds of nanocrystal LEDs but also is beneficial to the development of CQW-LEDs-based display technology and related integrated optoelectronics.

Advances in Perovskite Light-Emitting Diodes Possessing Improved Lifetime.

Recently, perovskite light-emitting diodes (PeLEDs) are seeing an increasing academic and industrial interest with a potential for a broad range of technologies including display, lighting, and signaling. The maximum external quantum efficiency of PeLEDs can overtake 20% nowadays, however, the lifetime of PeLEDs is still far from the demand of practical applications. In this review, state-of-the-art concepts to improve the lifetime of PeLEDs are comprehensively summarized from the perspective of the design of perovskite emitting materials, the innovation of device engineering, the manipulation of optical effects, and the introduction of advanced encapsulations. First, the fundamental concepts determining the lifetime of PeLEDs are presented. Then, the strategies to improve the lifetime of both organic-inorganic hybrid and all-inorganic PeLEDs are highlighted. Particularly, the approaches to manage optical effects and encapsulations for the improved lifetime, which are negligibly studied in PeLEDs, are discussed based on the related concepts of organic LEDs and Cd-based quantum-dot LEDs, which is beneficial to insightfully understand the lifetime of PeLEDs. At last, the challenges and opportunities to further enhance the lifetime of PeLEDs are introduced.