Uncooled Mid-Infrared Sensing Enabled by Chip-Integrated Low-Temperature-Grown 2D PdTe2 Dirac Semimetal.

Next-generation mid-infrared (MIR) imaging chips demand free-cooling capability and high-level integration. The rising two-dimensional (2D) semimetals with excellent infrared (IR) photoresponses are compliant with these requirements. However, challenges remain in scalable growth and substrate-dependence for on-chip integration. Here, we demonstrate the inch-level 2D palladium ditelluride (PdTe2) Dirac semimetal using a low-temperature self-stitched epitaxy (SSE) approach. The low formation energy between two precursors facilitates low-temperature multiple-point nucleation (∼300 °C), growing up, and merging, resulting in self-stitching of PdTe2 domains into a continuous film, which is highly compatible with back-end-of-line (BEOL) technology. The uncooled on-chip PdTe2/Si Schottky junction-based photodetector exhibits an ultrabroadband photoresponse of up to 10.6 µm with a large specific detectivity. Furthermore, the highly integrated device array demonstrates high-resolution room-temperature imaging capability, and the device can serve as an optical data receiver for IR optical communication. This study paves the way toward low-temperature growth of 2D semimetals for uncooled MIR sensing.

Strain effect on the field-effect sensing property of Si wires.

Silicon-based field effect transistor (FET) sensors with high sensitivity are emerging as powerful sensors for detecting chemical/biological species. Strain engineering has been demonstrated as an effective means to improve the performance of Si-based devices. However, the strain effect on the field-effect sensing property of silicon materials has not been studied yet. Here, we investigate the strain effect on the field-effect sensing property of silicon wires by taking humidity sensing as an example. The humidity sensitivity of FET sensors based on silicon wires increases with increasing tensile strain but decreases with increasing compressive strain. The sensitivity is very responsive to strain with an enhancement factor of 67 for tensile strain. Theoretical analysis shows that the sensitivity variation under different strains is mainly attributed to the change in adsorption energy between silicon wires and water molecules. This work indicates that strain engineering can be an effective route to modulate the field-effect sensing property of Si wires for constructing highly sensitive Si-based FET sensors.

Ultraminiaturized Stretchable Strain Sensors Based on Single Silicon Nanowires for Imperceptible Electronic Skins.

Miniaturized stretchable strain sensors are key components in E-skins for applications such as personalized health-monitoring, body motion perception, and human-machine interfaces. However, it remains a big challenge to fabricate miniaturized stretchable strain sensors with high imperceptibility. Here, we reported for the first time novel ultraminiaturized stretchable strain sensors based on single centimeter-long silicon nanowires (cm-SiNWs). With the diameter of the active materials even smaller than that of spider silks, these sensors are highly imperceptible. They exhibit a large strain sensing range (>45%) and a high durability (>10 000 cycles). Their optimum strain sensing ranges could be modulated by controlling the prestrains of the stretchable cm-SiNWs. On the basis of this capability, sensors with appropriate sensing ranges were chosen to respectively monitor large and subtle human motions including joint motion, swallow, and touch. The strategy of applying single cm-SiNWs in stretchable sensors would open new doors to fabricate ultraminiaturized stretchable devices.

Characterizing the Conformational Distribution in an Amorphous Film of an Organic Emitter and Its Application in a "Self-Doping" Organic Light-Emitting Diode.

The conformational distribution and mutual interconversion of thermally activated delayed fluorescence (TADF) emitters significantly affect the exciton utilization. However, their influence on the photophysics in amorphous film states is still not known due to the lack of a suitable quantitative analysis method. Herein, we used temperature-dependent time-resolved photoluminescence spectroscopy to quantitatively measure the relative populations of the conformations of a TADF emitter for the first time. We further propose a new concept of "self-doping" for realizing high-efficiency nondoped OLEDs. Interestingly, this "compositionally" pure film actually behaves as a film with a dopant (quasi-equatorial form) in a matrix (quasi-axial form). The concentration-induced quenching that may occur at high concentrations is thus expected to be effectively relieved. The "self-doping" OLED prepared with the newly developed TADF emitter TP2P-PXZ as a neat emitting layer realizes a high maximum external quantum efficiency of 25.4 % and neglectable efficiency roll-off.

Precise Patterning of Organic Semiconductor Crystals for Integrated Device Applications.

Development of high-performance organic electronic and optoelectronic devices relies on high-quality semiconducting crystals that have outstanding charge transport properties and long exciton diffusion length and lifetime. To achieve integrated device applications, it is a prerequisite to precisely locate the organic semiconductor crystals (OSCCs) to form a specifically patterned structure. Well-patterned OSCCs can not only reduce leakage current and cross-talk between neighboring devices, but also facilely integrate with other device elements and their corresponding interconnects. In this Review, general strategies for the patterning of OSCCs are summarized, and the advantages and limitations of different patterning methods are discussed. Discussion is focused on an advanced strategy for the high-resolution and wafer-scale patterning of OSCC by a surface microstructure-assisted patterning method. Furthermore, the recent progress on OSCC pattern-based integrated circuities is highlighted. Finally, the research challenges and directions of this young field are also presented.

Layer-Defining Strategy to Grow Two-Dimensional Molecular Crystals on a Liquid Surface down to the Monolayer Limit.

Two-dimensional molecular crystals (2DMCs) open a new door for the controllable growth of 2D materials by molecular design with a energy gap and solution processability. However, the growth of 2DMCs with defined molecular layers remains full of challenges. Herein, we report a novel method to produce various 2DMCs with a defined number of molecular layers. When the surface tension and viscosity are tuned to control the spreading of the solution on the liquid surface, large-area quasi-freestanding 2DMCs from bulk size down to the monolayer limit are obtained, which makes it possible to probe the intrinsic layer-dependent optoelectronic properties of organic semiconductors down to the physical limit, and paves the way for the application of 2DMCs in new optoelectronic devices and technologies.

Ultrahigh-Responsivity Photodetectors from Perovskite Nanowire Arrays for Sequentially Tunable Spectral Measurement.

Compared with polycrystalline films, single-crystalline methylammonium lead halide (MAPbX3, X = halogen) perovskite nanowires (NWs) with well-defined structure possess superior optoelectronic properties for optoelectronic applications. However, most of the prepared perovskite NWs exhibit properties below expectations due to poor crystalline quality and rough surfaces. It also remains a challenge to achieve aligned growth of single-crystalline perovskite NWs for integrated device applications. Here, we report a facile fluid-guided antisolvent vapor-assisted crystallization (FGAVC) method for large-scale fabrication of high-quality single-crystalline MAPb(I1-xBrx)3 (x = 0, 0.1, 0.2, 0.3, 0.4) NW arrays. The resultant perovskite NWs showed smooth surfaces due to slow crystallization process and moisture-isolated growth environment. Significantly, photodetectors made from the NW arrays exhibited outstanding performance in respect of ultrahigh responsivity of 12 500 A W-1, broad linear dynamic rang (LDR) of 150 dB, and robust stability. The responsivity represents the best value ever reported for perovskite-based photodetectors. Moreover, the spectral response of the MAPb(I1-xBrx)3 NW arrays could be sequentially tuned by varying the content of x = 0-0.4. On the basis of this feature, the NW arrays were monolithically integrated to form a unique system for directly measuring light wavelength. Our work would open a new avenue for the fabrication of high-performance, integrated optoelectronic devices from the perovskite NW arrays.

Centimeter-Long Single-Crystalline Si Nanowires.

The elongation of free-standing one-dimensional (1D) functional nanostructures into lengths above the millimeter range has brought new practical applications as they combine the remarkable properties of nanostructured materials with macroscopic lengths. However, it remains a big challenge to prepare 1D silicon nanostructures, one of the most important 1D nanostructures, with lengths above the millimeter range. Here we report the unprecedented preparation of ultralong single-crystalline Si nanowires with length up to 2 cm, which can function as the smallest active material to facilitate the miniaturization of macroscopic devices. These ultralong Si nanowires with augmented flexibility are of emerging interest for flexible electronics. We also demonstrate the first single-nanowire-based wearable joint motion sensor with superior performance to reported systems, which just represents one example of novel devices that can be built from these nanowires. The preparation of ultralong Si nanowires will stimulate the fabrication and miniaturization of electric, optical, medical, and mechanical devices to impact the semiconductor industry and our daily life in the near future.

Precise Patterning of Organic Single Crystals via Capillary-Assisted Alternating-Electric Field.

Owing to the extraordinary properties, organic micro/nanocrystals are important building blocks for future low-cost and high-performance organic electronic devices. However, integrated device application of the organic micro/nanocrystals is hampered by the difficulty in high-throughput, high-precision patterning of the micro/nanocrystals. In this study, the authors demonstrate, for the first time, a facile capillary-assisted alternating-electric field method for the large-scale assembling and patterning of both 0D and 1D organic crystals. These crystals can be precisely patterned at the photolithography defined holes/channels at the substrate with the yield up to 95% in 1 mm2 . The mechanism of assembly kinetics is systematically studied by the electric field distribution simulation and experimental investigations. By using the strategy, various organic micro/nanocrystal patterns are obtained by simply altering the geometries of the photoresist patterns on substrates. Moreover, ultraviolet photodetectors based on the patterned Alq3 micro/nanocrystals exhibit visible-blind photoresponse with high sensitivity as well as excellent stability and reproducibility. This work paves the way toward high-integration, high-performance organic electronic, and optoelectronic devices from the organic micro/nanocrystals.

On the Mechanism of Hydrophilicity of Graphene.

It is generally accepted that the hydrophilic property of graphene can be affected by the underlying substrate. However, the role of intrinsic vs substrate contributions and the related mechanisms are vividly debated. Here, we show that the intrinsic hydrophilicity of graphene can be intimately connected to the position of its Fermi level, which affects the interaction between graphene and water molecules. The underlying substrate, or dopants, can tune hydrophilicity by modulating the Fermi level of graphene. By shifting the Fermi level of graphene away from its Dirac point, via either chemical or electrical voltage doping, we show enhanced hydrophilicity with experiments and first principle simulations. Increased vapor condensation on graphene, induced by a simple shifting of its Fermi level, exemplifies applications in the area of interfacial transport phenomena.

MoO3 Nanodots Decorated CdS Nanoribbons for High-Performance, Homojunction Photovoltaic Devices on Flexible Substrates.

The p-n homojunctions are essential components for high-efficiency optoelectronic devices. However, the lack of p-type doping in CdS nanostructures hampers the fabrication of efficient photovoltaic (PV) devices from homojunctions. Here we report a facile solution-processed method to achieve efficient p-type doping in CdS nanoribbons (NRs) via a surface charge transfer mechanism by using spin-coated MoO3 nanodots (NDs). The NDs-decorated CdS NRs exhibited a hole concentration as high as 8.5 × 10(19) cm(-3), with the p-type conductivity tunable in a wide range of 7 orders of magnitude. The surface charge transfer mechanism was characterized in detail by X-ray photoelectron spectroscopy, Kelvin probe force microscopy, and first-principle calculations. CdS NR-homojunction PV devices fabricated on a flexible substrate exhibited a power conversion efficiency of 5.48%, which was significantly better than most of the CdS nanostructure-based heterojunction devices, presumably due to minimal junction defects. Devices made by connecting cells in series or in parallel exhibited enhanced power output, demonstrating the promising potential of the homojunction PV devices for device integration. Given the high efficiency of the surface charge transfer doping and the solution-processing capability of the method, our work opens up unique opportunities for high-performance, low-cost optoelectronic devices based on CdS homojunctions.

Macroscopic and Strong Ribbons of Functionality-Rich Metal Oxides from Highly Ordered Assembly of Unilamellar Sheets.

The strong interest in macroscopic graphene and/or carbon nanotube (CNT) fiber has highlighted that anisotropic nanostructured materials are ideal components for fabricating fiber assemblies. Prospectively, employing two-dimensional (2D) crystals or nanosheets of functionality-rich transition metal oxides would notably enrich the general knowledge for desirable fiber constructions and more importantly would greatly broaden the scope of functionalities. However, the fibers obtained up to now have been limited to carbon-related materials, while those made of 2D crystals of metal oxides have not been achieved, probably due to the intrinsically low mechanical stiffness of a molecular sheet of metal oxides, which is only few hundredths of that for graphene. Here, using 2D titania sheets as an illustrating example, we present the first successful fabrication of macroscopic fiber of metal oxides composed of highly aligned stacking sheets with enhanced sheet-to-sheet binding interactions. Regardless of the intrinsically weak Ti-O bond in molecular titania sheets, the optimal fiber manifested mechanical performance comparable to that documented for graphene or CNTs. This work provided important hints for devising optimized architecture in macroscopic assemblies, and the rich functionalities of titania promises fibers with limitless promise for a wealth of innovative applications.

Bilayer graphene based surface passivation enhanced nano structured self-powered near-infrared photodetector.

A simple methyl-terminated (-CH(3)) surface passivation approach has been employed to enhance the performance of the bilayer graphene/Si nanohole array (BLG/SiNH array) Schottky junction based self-powered near infrared photodetector (SPNIRPD). The as-fabricated SPNIRPD exhibits high sensitivity to light at near infrared region at zero bias voltage. The I(light)/I(dark) ratio measured is 1.43 × 10(7), which is more than an order of magnitude improvement compared with the sample without passivation (~6.4 × 10(5)). Its corresponding responsivity and detectivity are 0.328 AW(-1) and 6.03 × 10(13) cmHz(1/2)W(-1), respectively. The demonstrated results have confirmed the high-performance SPNIRPD compared with the photo-detectors of similar type and its great potential application in future optoelectronic devices.

Patterned growth of single-crystal 3, 4, 9, 10-perylenetetracarboxylic dianhydride nanowire arrays for field-emission and optoelectronic devices.

3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) organic nanostructures possess extraordinary electronic and optoelectronic properties. However, it remains a challenge to achieve patterned growth of PTCDA nanowire (NW) arrays for integrated device applications. Here, we demonstrated the high-density, large-area, uniform, and cross-aligned growth of single-crystalline PTCDA NW arrays by using Au nanoparticles (NPs) as the growth templates. The high surface energy of Au NPs led to the cross-aligned growth of organic NWs, enabling the growth of PTCDA NW arrays with any desirable patterns by pre-patterning the Au films on a Si substrate. The PTCDA NW arrays as field emitters show good performance with a large emission current density and high emission stability. Furthermore, photodetectors based on PTCDA NW arrays were constructed via a simple in-situ growth approach, which exhibited high sensitivity to a wideband light ranging from 400-800 nm and surpassed the individual NW-based photodetectors in terms of higher photocurrent and faster response speed. Successful applications of PTCDA NW arrays in field emission and photodetectors show a great potential application of organic NW arrays in future efficient electronic and optoelectronic devices.

Facile One-Step Fabrication of Ordered Ultra-Long Organic Microwires Film for Flexible Near-Infrared Photodetectors.

Micro/nanoscale electronic devices, such as transistors and sensors, made from single-crystalline organic micro/nano-structures with tunable molecular/structural design are much smaller and more versatile than those that rely on conventional polycrystalline/amorphous organic films, but their development for mass production has been thwarted by difficulties in aligning and integrating the organic crystals required. Here, we developed an improved evaporation induced self-assemble method to accomplish large-area uniform growth of ultra-long methyl-squarylium (MeSq) microwires (MWs) films. The MWs could align along the dewetting direction of the solution with length over the entire substrate, thus lessening the requirement for precisely addressing the positions of MWs. Near infrared (NIR) photodetectors based on the ordered organic MWs film were directly constructed on Si/SiO2 substrate. The MeSq MWs showed high sensitivity to the NIR light with excellent stability and repeatability. To evaluate the potential applications of the organic MWs film in flexible and transparent electronics, flexible photodetectors were constructed by transferring the MWs film to polydimethylsiloxane (PDMS) substrate. Significantly, the device showed good flexibility and could stand a large bending stress due to the superior mechanical flexibility of the organic MWs. This characteristic opens new prospects for the applications of the MeSq MWs.

Freestanding Serpentine Silicon Strips with Ultrahigh Stretchability over 300% for Wearable Electronics.

Well-functionalized electronic materials, such as silicon, in a stretchable format are desirable for high-performance wearable electronics. However, obtaining Si materials that meet the required stretchability of over 100% for wearable applications remains a significant challenge. Herein, a rational design strategy is proposed to achieve freestanding serpentine Si strips (FS-Si strips) with ultrahigh stretchability, fulfilling wearable requirements. The self-supporting feature makes the strips get rid of excessive constraints from substrates and enables them to deform with the minimum strain energy. Micrometer-scale thicknesses enhance robustness, and large diameter-to-width ratios effectively reduce strain concentration. Consequently, the FS-Si strips with the optimum design could withstand 300% stretch, bending, and torsion without fracturing, even under rough manual operation. They also exhibit excellent stability and durability over 50,000 cycles of 100% stretching cycles. For wearable applications, the FS-Si strips can maintain conformal contact with the skin and have a maximum stretchability of 120%. Moreover, they are electrically insensitive to large deformations, which ensure signal stability during their daily use. Combined with mature processing techniques and the excellent semiconductor properties of Si, FS-Si strips are promising core stretchable electronic materials for wearable electronics.

Breaking Fundamental Limitation of Flow-Induced Anisotropic Growth for Large-Scale and Fast Printing of Organic Single-Crystal Films.

Advanced organic electronic technologies have put forward a pressing demand for cost-effective and high-throughput fabrication of organic single-crystal films (OSCFs). However, solution-printed OSCFs are typically plagued by the existence of abundant structural defects, which pose a formidable challenge to achieving large-scale and high-performance organic electronics. Here, it is elucidated that these structural defects are mainly originated from printing flow-induced anisotropic growth, an important factor that is overlooked for too long. In light of this, a surfactant-additive printing method is proposed to effectively overcome the anisotropic growth, enabling the deposition of uniform OSCFs over the wafer scale at a high speed of 1.2 mm s-1 at room temperature. The resulting OSCF exhibits appealing performance with a high average mobility up to 10.7 cm2 V-1 s-1, which is one of the highest values for flexible organic field-effect transistor arrays. Moreover, large-scale OSCF-based flexible logic circuits, which can be bent without degradation to a radius as small as 4.0 mm and over 1000 cycles are realized. The work provides profound insights into breaking the limitation of flow-induced anisotropic growth and opens new avenues for printing large-scale organic single-crystal electronics.

A floating-gate field-effect transistor memory device based on organic crystals with a built-in tunneling dielectric by a one-step growth strategy.

A floating-gate organic field-effect transistor (FG-OFET) memory device is becoming a promising candidate for emerging non-volatile memory applications due to the advantages of its sophisticated data-storage mechanism and reliable long-term data retention capacity. However, a conventional FG-OFET memory device suffers from complex fabrication technologies and poor mechanical flexibility, which limits its practical applications. Here, we propose a facile one-step liquid-surface drag coating strategy to fabricate a layered stack of 2,8-difluoro-5,11-bis(triethylsilylethynyl) anthradithiophene (Dif-TES-ADT) crystals and high-quality insulating polymer polystyrene (PS). The liquid surface enhances the spreading area of an organic solution and facilitates the unidirectional growth of organic crystals. In the bilayer-structured blend, the bottom PS polymer and the top Dif-TES-ADT semiconductor serve as a tunneling dielectric and an active memory layer of an FG-OFET memory device, respectively. Consequently, a flexible FG-OFET memory device with a large memory window of 41.4 V, a long retention time of 5000 s, and a high current ON/OFF ratio of 105 could be achieved, showing the best performance ever reported for organic thin film-based FG-OFET memory devices. In addition, multi-level data storage (3 bits per cell) can be achieved by tuning the gate voltage magnitude. Our work not only provides a general strategy for the growth of high-quality organic crystals, but also paves the way towards high-performance flexible memory devices.

Bionic Scotopic Adaptation Transistors for Nighttime Low Illumination Imaging.

Human vision excels in perceiving nighttime low illumination due to biological feedforward adaptation. Replicating this ability in biomimetic vision using solid-state devices has been highly sought after. However, emulating scotopic adaptation, entailing a confluence of efficient photoexcitation and dynamic carrier modulation, presents formidable challenges. Here, we demonstrate a low-power and bionic scotopic adaptation transistor by coupling a light-absorption layer and an electron-trapping layer at the bottom of the semiconducting channel, enabling simultaneous achievement of efficient generation of free photocarriers and adaptive carrier accumulation within a single device. This innovation empowers our transistor to exhibit sensitivity-potentiated characteristics after adaptation, detecting scotopic-level illumination (0.001 lx) with exceptional photosensitivity up to 103 at low voltages below 2 V. Moreover, we have successfully replicated diverse scotopic vision functions, encompassing time-dependent visual threshold enhancement, light intensity-dependent adaptation index, imaging contrast enhancement for nighttime low illumination imaging, opening an opportunity for artificial night vision.

Monolayer graphene film on ZnO nanorod array for high-performance Schottky junction ultraviolet photodetectors.

A new Schottky junction ultraviolet photodetector (UVPD) is fabricated by coating a free-standing ZnO nanorod (ZnONR) array with a layer of transparent monolayer graphene (MLG) film. The single-crystalline [0001]-oriented ZnONR array has a length of about 8-11 µm, and a diameter of 100∼600 nm. Finite element method (FEM) simulation results show that this novel nanostructure array/MLG heterojunction can trap UV photons effectively within the ZnONRs. By studying the I-V characteristics in the temperature range of 80-300 K, the barrier heights of the MLG film/ZnONR array Schottky barrier are estimated at different temperatures. Interestingly, the heterojunction diode with typical rectifying characteristics exhibits a high sensitivity to UV light illumination and a quick response of millisecond rise time/fall times with excellent reproducibility, whereas it is weakly sensitive to visible light irradiation. It is also observed that this UV photodetector (PD) is capable of monitoring a fast switching light with a frequency as high as 2250 Hz. The generality of the above results suggest that this MLG film/ZnONR array Schottky junction UVPD will have potential application in future optoelectronic devices.