Spectrum Reconstruction with Filter-Free Photodetectors Based on Graded-Band-Gap Perovskite Quantum Dot Heterojunctions.

Spectrum reconstruction with filter-free microspectrometers has attracted much attention owing to their promising potential in in situ analysis systems, on-chip spectroscopy characterizations, hyperspectral imaging, etc. Further efforts in this field can be devoted to improving the performance of microspectrometers by employing high-performance photosensitive materials and optimizing the reconstruction algorithms. In this work, we demonstrate spectrum reconstruction with a set of photodetectors based on graded-band-gap perovskite quantum dot (PQD) heterojunctions using both calculation and machine learning algorithms. The photodetectors exhibit good photosensitivities with nonlinear current-voltage curves, and the devices with different PQD band gaps show various spectral responsivities with different cutoff wavelength edges covering the entire visible range. Reconstruction performances of monochromatic spectra with the set of PQD photodetectors using two different algorithms are compared, and the machine learning method achieves relatively better accuracy. Moreover, the nonlinear current-voltage variation of the photodetectors can provide increased data diversity without redundancy, thus further improving the accuracy of the reconstructed spectra for the machine learning algorithm. A spectral resolution of 10 nm and reconstruction of multipeak spectra are also demonstrated with the filter-free photodetectors. Therefore, this study provides PQD photodetectors with the corresponding optimized algorithms for emerging flexible microspectrometer systems.

Power-Efficient Gas-Sensing and Synaptic Diodes Based on Lateral Pentacene/a-IGZO PN Junctions.

Function convergence of gas sensing and neuromorphic computing is attracting much research attention due to the promising potential in electronic olfactory, artificial intelligence, and internet of everything systems. However, the current neuromorphic gas-sensing systems are either realized via integration of gas detectors and neuromorphic devices or operating with three-terminal synaptic transistors at high voltages, leading to a rather high system complexity or power consumption. Herein, gas-modulated synaptic diodes with lateral structures are developed to converge sensing, processing, and storage functions into a single device. The lateral synaptic diode is based on a p-n junction of an organic semiconductor (OSC) and amorphous In-Ga-Zn-O, in which the upper OSC layer can directly interact with the gas molecules in the atmosphere. Typical synaptic behaviors triggered by ammonia, including inhibitory postsynaptic current and paired-pulse depression, are successfully demonstrated. Meanwhile, a low power consumption of 6.3 pJ per synaptic event has been achieved, which benefits from the simple device structure, the decent chemosensitivity of the OSC, and the low operation voltage. A simulated ammonia analysis in human exhaled breath is further conducted to explore the practical application of the synaptic diode. Therefore, this work provides a gas-modulated synaptic diode for circuit-compact and power-efficient artificial olfactory systems.

Efficient and Stable Perovskite Photodetectors Based on Thiocyanate-Assisted Film Formation.

Thiocyanate-based perovskite (SCN-PVSK) photodetectors have been fabricated by introducing lead thiocyanate precursor. Incorporating SCN groups into CH3NH3PbI3 can significantly improve the device stability in air. Compared with pure CH3NH3PbI3 films, SCN-PVSK films have larger grain size and reduced trap states. The perovskite layers can be prepared by a simple solution method in air. Solvent effects on the crystallization of SCN-PVSK films have also been investigated. It is found that highly uniform, pinhole-free perovskite films can be obtained utilizing the N,N-dimethylformamide (DMF) solution of Pb(SCN)2. The SCN-PVSK based photodetectors performed a high responsivity of 12.3 A/W and a decent detectivity over 1.3 × 1013 Jones. More important, the SCN-PVSK based two-terminal photodetectors, without encapsulation, have shown great stability with 92% of the initial photocurrent being retained after storage in air (relative humidity >50%) for 10 days, whereas the value is only 10% for pure CH3NH3PbI3 devices tested under the same conditions.

Gas Sensors Based on Nano/Microstructured Organic Field-Effect Transistors.

Benefiting from the advantages of organic field-effect transistors (OFETs), including synthetic versatility of organic molecular design and environmental sensitivity, gas sensors based on OFETs have drawn much attention in recent years. Potential applications focus on the detection of specific gas species such as explosive, toxic gases, or volatile organic compounds (VOCs) that play vital roles in environmental monitoring, industrial manufacturing, smart health care, food security, and national defense. To achieve high sensitivity, selectivity, and ambient stability with rapid response and recovery speed, the regulation and adjustment of the nano/microstructure of the organic semiconductor (OSC) layer has proven to be an effective strategy. Here, the progress of OFET gas sensors with nano/microstructure is selectively presented. Devices based on OSC films one dimensional (1D) single crystal nanowires, nanorods, and nanofibers are introduced. Then, devices based on two dimensional (2D) and ultrathin OSC films, fabricated by methods such as thermal evaporation, dip-coating, spin-coating, and solution-shearing methods are presented, followed by an introduction of porous OFET sensors. Additionally, the applications of nanostructured receptors in OFET sensors are given. Finally, an outlook in view of the current research state is presented and eight further challenges for gas sensors based on OFETs are suggested.

Hybrid Field-Effect Transistors and Photodetectors Based on Organic Semiconductor and CsPbI3 Perovskite Nanorods Bilayer Structure.

The outstanding performances of nanostructured all-inorganic CsPbX3 (X = I, Br, Cl) perovskites in optoelectronic applications can be attributed to their unique combination of a suitable bandgap, high absorption coefficient, and long carrier lifetime, which are desirable for photodetectors. However, the photosensing performances of the CsPbI3 nanomaterials are limited by their low charge-transport efficiency. In this study, a phototransistor with a bilayer structure of an organic semiconductor layer of 2,7-dioctyl [1] benzothieno[3,2-b] [1] benzothiophene and CsPbI3 nanorod layer was fabricated. The high-quality CsPbI3 nanorod layer obtained using a simple dip-coating method provided decent transistor performance of the hybrid transistor device. The perovskite layer efficiently absorbs light, while the organic semiconductor layer acts as a transport channel for injected photogenerated carriers and provides gate modulation. The hybrid phototransistor exhibits high performance owing to the synergistic function of the photogating effect and field effect in the transistor, with a photoresponsivity as high as 4300 A W-1, ultra-high photosensitivity of 2.2 × 106, and excellent stability over 1 month. This study provides a strategy to combine the advantages of perovskite nanorods and organic semiconductors in fabrication of high-performance photodetectors.

Intrinsically ionic conductive cellulose nanopapers applied as all solid dielectrics for low voltage organic transistors.

Biodegradability, low-voltage operation, and flexibility are important trends for the future organic electronics. High-capacitance dielectrics are essential for low-voltage organic field-effect transistors. Here we report the application of environmental-friendly cellulose nanopapers as high-capacitance dielectrics with intrinsic ionic conductivity. Different with the previously reported liquid/electrolyte-gated dielectrics, cellulose nanopapers can be applied as all-solid dielectrics without any liquid or gel. Organic field-effect transistors fabricated with cellulose nanopaper dielectrics exhibit good transistor performances under operation voltage below 2 V, and no discernible drain current change is observed when the device is under bending with radius down to 1 mm. Interesting properties of the cellulose nanopapers, such as ionic conductivity, ultra-smooth surface (~0.59 nm), high transparency (above 80%) and flexibility make them excellent candidates as high-capacitance dielectrics for flexible, transparent and low-voltage electronics.

A flexible ionic synaptic device and diode-based aqueous ion sensor utilizing asymmetric polyelectrolyte distribution.

This work reported the development of an ionic diode of high rectification ratio with a simple device structure and a quick fabrication process by utilizing asymmetric polyelectrolyte distribution. Detection of aqueous ions was demonstrated by applying this diode as a pH sensor. Two terminal ionic synaptic devices utilizing a similar structural design were also successfully developed.

Light-Stimulated Synaptic Devices Utilizing Interfacial Effect of Organic Field-Effect Transistors.

Synaptic transistors stimulated by light waves or photons may offer advantages to the devices, such as wide bandwidth, ultrafast signal transmission, and robustness. However, previously reported light-stimulated synaptic devices generally require special photoelectric properties from the semiconductors and sophisticated device's architectures. In this work, a simple and effective strategy for fabricating light-stimulated synaptic transistors is provided by utilizing interface charge trapping effect of organic field-effect transistors (OFETs). Significantly, our devices exhibited highly synapselike behaviors, such as excitatory postsynaptic current (EPSC) and pair-pulse facilitation (PPF), and presented memory and learning ability. The EPSC decay, PPF curves, and forgetting behavior can be well expressed by mathematical equations for synaptic devices, indicating that interfacial charge trapping effect of OFETs can be utilized as a reliable strategy to realize organic light-stimulated synapses. Therefore, this work provides a simple and effective strategy for fabricating light-stimulated synaptic transistors with both memory and learning ability, which enlightens a new direction for developing neuromorphic devices.

Distinguishable Detection of Ultraviolet, Visible, and Infrared Spectrum with High-Responsivity Perovskite-Based Flexible Photosensors.

Distinguishable detection of the ultraviolet, visible, and infrared spectrum is promising and significant for the super visual system of artificial intelligences. However, it is challenging to provide a photosensor with such broad spectral response ability. In this work, the ultraviolet, visible, and infrared spectrum is distinguished by developing serial photosensors based on perovskite/carbon nanotube hybrids. Oraganolead halide perovskites (CH3 NH3 PbX3 ) possess remarkable optoelectronic properties and tunable optical band gaps by changing the halogens, and integration with single-walled carbon nanotubes can further improve their photoresponsivities. The CH3 NH3 PbCl3 -based photosensor shows a responsivity up to 105 A W-1 to ultraviolet and no obvious response to visible light, which is superior to that of most ultraviolet sensors. The CH3 NH3 PbBr3 -based photosensor exhibits a high responsivity to visible light. Serial devices of the two hybrid photosensors with comparable electric and sensory performances can distinguish the spectrum of ultraviolet, visible, and infrared even with varying light intensities. The photosensors also demonstrate excellent mechanical flexibility and bending stability. By taking full advantages of the oraganolead halide perovskites, this work provides flexible high-responsivity photosensors specialized for ultraviolet, and gives a simple strategy for distinguishable detection of ultraviolet, visible, and infrared spectrum based on the serial flexible photosensors.

Pursuing Polymer Dielectric Interfacial Effect in Organic Transistors for Photosensing Performance Optimization.

Polymer dielectrics in organic field-effect transistors (OFETs) are essential to provide the devices with overall flexibility, stretchability, and printability and simultaneously introduce charge interaction on the interface with organic semiconductors (OSCs). The interfacial effect between various polymer dielectrics and OSCs significantly and intricately influences device performance. However, understanding of this effect is limited because the interface is buried and the interfacial charge interaction is difficult to stimulate and characterize. Here, this challenge is overcome by utilizing illumination to stimulate the interfacial effect in various OFETs and to characterize the responses of the effect by measuring photoinduced changes of the OFETs performances. This systemic investigation reveals the mechanism of the intricate interfacial effect in detail, and mathematically explains how the photosensitive OFETs characteristics are determined by parameters including polar group of the polymer dielectric and the OSC side chain. By utilizing this mechanism, performance of organic electronics can be precisely controlled and optimized. OFETs with strong interfacial effect can also show a signal additivity caused by repeated light pulses, which is applicable for photostimulated synapse emulator. Therefore, this work enlightens a detailed understanding on the interface effect and provides novel strategies for optimizing OFET photosensory performances.

High-Performance Inorganic Perovskite Quantum Dot-Organic Semiconductor Hybrid Phototransistors.

All-inorganic lead halide perovskite quantum dots (IHP QDs) have great potentials in photodetectors. However, the photoresponsivity is limited by the low charge transport efficiency of the IHP QD layers. High-performance phototransistors based on IHP QDs hybridized with organic semiconductors (OSCs) are developed. The smooth surface of IHP QD layers ensures ordered packing of the OSC molecules above them. The OSCs significantly improve the transportation of the photoexcited charges, and the gate effect of the transistor structure significantly enhances the photoresponsivity while simultaneously maintaining high Iphoto /Idark ratio. The devices exhibit outstanding optoelectronic properties in terms of photoresponsivity (1.7 × 104 A W-1 ), detectivity (2.0 × 1014 Jones), external quantum efficiency (67000%), Iphoto /Idark ratio (8.1 × 104 ), and stability (100 d in air). The overall performances of our devices are superior to state-of-the-art IHP photodetectors. The strategy utilized here is general and can be easily applied to many other perovskite photodetectors.

Direct Detection of Dilute Solid Chemicals with Responsive Lateral Organic Diodes.

Organic field-effect transistors (OFETs) have emerged as promising sensors targeting chemical analytes in vapors and liquids. However, the direct detection of solid chemicals by OFETs has not been achieved. Here for the first time, we describe the direct detection of solid chemical analytes by organic electronics. An organic diode structure based on a horizontal side-by-side p-n junction was adopted and shown to be superior to OFETs for this purpose. The diodes showed more than 40% current decrease upon exposure to 1 ppm melamine powders. The estimated detection limit to melamine can potentially reach the ppb range. This is the first demonstration of an electronic signal from an interaction between a solid and an organic p-n junction directly, which suggests that our lateral organic diodes are excellent platforms for the development of future sensors when direct detection of solid chemicals is needed. The approach developed here is general and can be extended to chemical sensors targeting various analytes, opening unprecedented opportunities for the development of low-cost and high-performance solid chemical sensors.

Preparation of Advanced CuO Nanowires/Functionalized Graphene Composite Anode Material for Lithium Ion Batteries.

The copper oxide (CuO) nanowires/functionalized graphene (f-graphene) composite material was successfully composed by a one-pot synthesis method. The f-graphene synthesized through the Birch reduction chemistry method was modified with functional group "-(CH2)5COOH", and the CuO nanowires (NWs) were well dispersed in the f-graphene sheets. When used as anode materials in lithium-ion batteries, the composite exhibited good cyclic stability and decent specific capacity of 677 mA·h·g-1 after 50 cycles. CuO NWs can enhance the lithium-ion storage of the composites while the f-graphene effectively resists the volume expansion of the CuO NWs during the galvanostatic charge/discharge cyclic process, and provide a conductive paths for charge transportation. The good electrochemical performance of the synthesized CuO/f-graphene composite suggests great potential of the composite materials for lithium-ion batteries anodes.

Facile Synthesis of a MoS2 and Functionalized Graphene Heterostructure for Enhanced Lithium-Storage Performance.

A facile strategy was designed for the in situ synthesis of MoS2 nanospheres on functionalized graphene nanoplates (MoS2@f-graphene) for use as lithium-ion battery anode materials. A modified Birch reduction was used to exfoliate graphite into few-layer graphene followed by modification with functional groups. Compared to the most common approach of mixing MoS2 and reduced graphene oxide, our approach provides a way to circumvent the harsh oxidation and destruction of the carbon basal planes. In this process, alkylcarboxyl functional groups on the functionalized graphene (f-graphene) serve as sites where MoS2 nanospheres crystallize, and thus create bridges between the MoS2 nanospheres and the graphene layers to effectively facilitate electronic transport and to avoid both the aggregation of MoS2 and the restacking of graphene. As anode materials, this unique MoS2@f-graphene heterostructure has a high specific capacity of 1173 mAh g-1 at a current density of 100 mA g-1 and a good rate capacity (910 mAh g-1 at 1600 mA g-1).

Photosensitive and Flexible Organic Field-Effect Transistors Based on Interface Trapping Effect and Their Application in 2D Imaging Array.

Flexible organic phototransistors are fabricated using polylactide (PLA), a polar bio-material, as the dielectric material. The charge trapping effect induced by the polar groups of the PLA layer leads to a photosensitivity close to ≈104. The excellent performance of this new device design is further demonstrated by incorporating the photo-transistors into a sensor array to successfully image a star pattern.

Photodetectors Based on Two-Dimensional Layer-Structured Hybrid Lead Iodide Perovskite Semiconductors.

Hybrid lead iodide perovskite semiconductors have attracted intense research interests recently because of their easy fabrication processes and high power conversion efficiencies in photovoltaic applications. Layer-structured materials have interesting properties such as quantum confinement effect and tunable band gap due to the unique two-dimensional crystalline structures. ⟨100⟩-oriented layer-structured perovskite materials are inherited from three-dimensional ABX3 perovskite materials with a generalized formula of (RNH3)2(CH3NH3)n-1MnX3n+1, and adopt the Ruddlesden-Popper type crystalline structure. Here we report the synthesis and investigation of three layer-structured perovskite materials with different layer numbers: (C4H9NH3)2PbI4 (n = 1, one-layered perovskite), (C4H9NH3)2(CH3NH3)Pb2I7 (n = 2, two-layered perovskite) and (C4H9NH3)2(CH3NH3)2Pb3I10 (n = 3, three-layered perovskite). Their photoelectronic properties were investigated in related to their molecular structures. Photodetectors based on these two-dimensional (2D) layer-structured perovskite materials showed tunable photoresponse with short response time in milliseconds. The photodetectors based on three-layered perovskite showed better performances than those of the other two devices, in terms of output current, responsivity, Ilight/Idark ratio, and response time, because of its smaller optical band gap and more condensed microstructure comparing the other two materials. These results revealed the relationship between the molecular structures, film microstructures and the photoresponse properties of 2D layer-structured hybrid perovskites, and demonstrated their potentials as flexible, functional, and tunable semiconductors in optoelectronic applications, by taking advantage of their tunable quantum well molecular structure.

Ultrasensitive Photodetectors Based on Island-Structured CH3NH3PbI3 Thin Films.

CH3NH3PbI3 perovskite-based optoelectronics have attracted intense research interests recently because of their easy fabrication process and high power conversion efficiency. Herein, we report a novel photodetector based on unique CH3NH3PbI3 perovskite films with island-structured morphology. The light-induced electronic properties of the photodetectors were investigated and compared to those devices based on conventional compact CH3NH3PbI3 films. The island-structured CH3NH3PbI3 photodetectors exhibited a rapid response speed (<50 ms), good stability at a temperature of up to 100 °C, a large photocurrent to dark current ratio (Ilight/Idark > 1 × 10(4) under an incident light of ∼6.59 mW/cm(2), and Ilight/Idark > 1 × 10(2) under low incident light ∼0.018 mW/cm(2)), and excellent reproducibility. Especially, the performance of the island-structured devices markedly exceed that of the conventional compact CH3NH3PbI3 thin-film devices. These excellent performances render the island-structured device to be potentially applicable for a wide range of optoelectronics.