Wafer-Scale Fabrication of Wearable All-Carbon Nanotube Photodetector Arrays.

With electronic devices evolving toward portable and high-performance wearables, the constraints of complex and wet processing technologies become apparent. This study presents a scalable photolithography/chemical-free method for crafting wearable all-carbon nanotube (CNT) photodetector device arrays. Laser-assisted patterning and dry deposition techniques directly assemble gas-phase CNTs into flexible devices without any lithography or lift-off processes. The resulting wafer-scale all-CNT photodetector arrays showcase excellent uniformity, wearability, environmental stability, and notable broadband photoresponse, boasting a high responsivity of 44 AW-1 and a simultaneous detectivity of 1.9 × 109 Jones. This research provides an efficient, versatile, and scalable strategy for manufacturing wearable all-CNT device arrays, allowing widespread adoption in wearable optoelectronics and multifunctional sensors.

Highly Sensitive MoS2 Photodetectors Enabled with a Dry-Transferred Transparent Carbon Nanotube Electrode.

Fabricating electronic and optoelectronic devices by transferring pre-deposited metal electrodes has attracted considerable attention, owing to the improved device performance. However, the pre-deposited metal electrode typically involves complex fabrication procedures. Here, we introduce our facile electrode fabrication process which is free of lithography, lift-off, and reactive ion etching by directly press-transferring a single-walled carbon nanotube (SWCNT) film. We fabricated Schottky diodes for photodetector applications using dry-transferred SWCNT films as the transparent electrode to increase light absorption in photoactive MoS2 channels. The MoS2 flake vertically stacked with an SWCNT electrode can exhibit excellent photodetection performance with a responsivity of ∼2.01 × 103 A/W and a detectivity of ∼3.2 × 1012 Jones. Additionally, we carried out temperature-dependent current-voltage measurement and Fowler-Nordheim (FN) plot analysis to explore the dominant charge transport mechanism. The enhanced photodetection in the vertical configuration is found to be attributed to the FN tunneling and internal photoemission of charge carriers excited from indium tin oxide across the MoS2 layer. Our study provides a novel concept of using a photoactive MoS2 layer as a tunneling layer itself with a dry-transferred transparent SWCNT electrode for high-performance and energy-efficient optoelectronic devices.

Deterministic Light-to-Voltage Conversion with a Tunable Two-Dimensional Diode.

Heterojunctions accompanied by energy barriers are of significant importance in two-dimensional materials-based electronics and optoelectronics. They provide more functional device performance, compared with their counterparts with uniform channels. Multimodal optoelectronic devices could be accomplished by elaborately designing band diagrams and architectures of the two-dimensional junctions. Here, we demonstrate deterministic light-to-voltage conversion based on strong dielectric screening effect in a tunable two-dimensional Schottky diode based on semiconductor/metal heterostructure, where the resultant photovoltage is dependent on the intensity of light input but independent of gate voltage. The converted photovoltage across the diode is independent of gate voltage under both monochromatic laser and white light illumination. In addition, the Fermi level of two-dimensional semiconductor area on dielectric SiO2 is highly gate-dependent, leading to the tunable rectifying effect of this heterostructure, which corporates a vertical Schottky junction and a lateral homojunction. As a result, a constant open-circuit voltage of ∼0.44 V and a hybrid "photovoltaic + photoconduction" photoresponse behavior are observed under 1 µW illumination of 403 nm laser, in addition to an electrical rectification ratio up to nearly 104. The scanning photocurrent mappings under different bias voltages indicate that the switchable operation mode (photovoltaic, photoconduction, or hybrid) depends on the bias-dependent effective energy barrier at the two-dimensional semiconductor-metal interface. This approach provides a facile and reliable solution for deterministic on-chip light-to-voltage conversion and optical-to-electrical interconnects.

On-chip photonics and optoelectronics with a van der Waals material dielectric platform.

During the last few decades, photonic integrated circuits have increased dramatically, facilitating many high-performance applications, such as on-chip sensing, data processing, and inter-chip communications. The currently dominating material platforms (i.e., silicon, silicon nitride, lithium niobate, and indium phosphide), which have exhibited great application successes, however, suffer from their own disadvantages, such as the indirect bandgap of silicon for efficient light emission, and the compatibility challenges of indium phosphide with the silicon industry. Here, we report a new dielectric platform using nanostructured bulk van der Waals materials. On-chip light propagation, emission, and detection are demonstrated by taking advantage of different van der Waals materials. Low-loss passive waveguides with MoS2 and on-chip light sources and photodetectors with InSe have been realised. Our proof-of-concept demonstration of passive and active on-chip photonic components endorses van der Waals materials for offering a new dielectric platform with a large material-selection degree of freedom and unique properties toward close-to-atomic scale manufacture of on-chip photonic and optoelectronic devices.

Switchable Photoresponse Mechanisms Implemented in Single van der Waals Semiconductor/Metal Heterostructure.

van der Waals (vdW) heterostructures based on two-dimensional (2D) semiconducting materials have been extensively studied for functional applications, and most of the reported devices work with sole mechanism. The emerging metallic 2D materials provide us new options for building functional vdW heterostructures via rational band engineering design. Here, we investigate the vdW semiconductor/metal heterostructure built with 2D semiconducting InSe and metallic 1T-phase NbTe2, whose electron affinity χInSe and work function ΦNbTe2 almost exactly align. Electrical characterization verifies exceptional diode-like rectification ratio of >103 for the InSe/NbTe2 heterostructure device. Further photocurrent mappings reveal the switchable photoresponse mechanisms of this heterostructure or, in other words, the alternative roles that metallic NbTe2 plays. Specifically, this heterostructure device works in a photovoltaic manner under reverse bias, whereas it turns to phototransistor with InSe channel and NbTe2 electrode under high forward bias. The switchable photoresponse mechanisms originate from the band alignment at the interface, where the band bending could be readily adjusted by the bias voltage. In addition, a conceptual optoelectronic logic gate is proposed based on the exclusive working mechanisms. Finally, the photodetection performance of this heterostructure is represented by an ultrahigh responsivity of ∼84 A/W to 532 nm laser. Our results demonstrate the valuable application of 2D metals in functional devices, as well as the potential of implementing photovoltaic device and phototransistor with single vdW heterostructure.

Tunable Quantum Tunneling through a Graphene/Bi2Se3 Heterointerface for the Hybrid Photodetection Mechanism.

Graphene-based van der Waals heterostructures are promising building blocks for broadband photodetection because of the gapless nature of graphene. However, their performance is mostly limited by the inevitable trade-off between low dark current and photocurrent generation. Here, we demonstrate a hybrid photodetection mode based on the photogating effect coupled with the photovoltaic effect via tunable quantum tunneling through the unique graphene/Bi2Se3 heterointerface. The tunneling junction formed between the semimetallic graphene and the topologically insulating Bi2Se3 exhibits asymmetric rectifying and hysteretic current-voltage characteristics, which significantly suppresses the dark current and enhances the photocurrent. The photocurrent-to-dark current ratio increases by about a factor of 10 with the electrical tuning of tunneling resistance for efficient light detection covering the major photonic spectral band from the visible to the mid-infrared ranges. Our findings provide a novel concept of using tunable quantum tunneling for highly sensitive broadband photodetection in mixed-dimensional van der Waals heterostructures.

Single-step chemical vapour deposition of anti-pyramid MoS2/WS2 vertical heterostructures.

Van der Waals heterostructures are the fundamental building blocks of electronic and optoelectronic devices. Here we report that, through a single-step chemical vapour deposition (CVD) process, high-quality vertical bilayer MoS2/WS2 heterostructures with a grain size up to ∼60 µm can be synthesized from molten salt precursors, Na2MoO4 and Na2WO4. Instead of normal pyramid vertical heterostructures grown by CVD, this method synthesizes an anti-pyramid MoS2/WS2 structure, which is characterized by Raman, photoluminescence and second harmonic generation microscopy. Our facile CVD strategy for synthesizing anti-pyramid structures unveils a new synthesis route for the products of two-dimensional heterostructures and their devices for application.

Dual-gated mono-bilayer graphene junctions.

A lateral junction with an atomically sharp interface is extensively studied in fundamental research and plays a key role in the development of electronics, photonics and optoelectronics. Here, we demonstrate an electrically tunable lateral junction at atomically sharp interfaces between dual-gated mono- and bilayer graphene. The transport properties of the mono-bilayer graphene interface are systematically investigated with I ds-V ds curves and transfer curves, which are measured with bias voltage V ds applied in opposite directions across the asymmetric mono-bilayer interface. Nearly 30% difference between the output I ds-V ds curves of graphene channels measured at opposite V ds directions is observed. Furthermore, the measured transfer curves confirm that the conductance difference of graphene channels greatly depends on the doping level, which is determined by dual-gating. The V ds direction dependent conductance difference indicates the existence of a gate tunable junction in the mono-bilayer graphene channel, due to different band structures of monolayer graphene with zero bandgap and bilayer graphene with a bandgap opened by dual-gating. Simulation of the I ds-V ds curves based on a new numerical model validates the gate tunable junction at the mono-bilayer graphene interface from another point of view. The dual-gated mono-bilayer graphene junction and new protocol for I ds-V ds curve simulation pave a possible way for functional applications of graphene in next-generation electronics.

Magnetic Actuation of Flexible Microelectrode Arrays for Neural Activity Recordings.

Implantable microelectrodes that can be remotely actuated via external fields are promising tools to interface with biological systems at a high degree of precision. Here, we report the development of flexible magnetic microelectrodes (FMµEs) that can be remotely actuated by magnetic fields. The FMµEs consist of flexible microelectrodes integrated with dielectrically encapsulated FeNi (iron-nickel) alloy microactuators. Both magnetic torque- and force-driven actuation of the FMµEs have been demonstrated. Nanoplatinum-coated FMµEs have been applied for in vivo recordings of neural activities from peripheral nerves and cerebral cortex of mice. Moreover, owing to their ultrasmall sizes and mechanical compliance with neural tissues, chronically implanted FMµEs elicited greatly reduced neuronal cell loss in mouse brain compared to conventional stiff probes. The FMµEs open up a variety of new opportunities for electrically interfacing with biological systems in a controlled and minimally invasive manner.

Acceptor-free photomultiplication-type organic photodetectors.

A series of organic photodetectors (OPDs) is prepared with two donor materials as active layers, with the only difference being the weight ratio of the two donors (one polymer and one small molecule). The OPDs work according to a photodiode model with an external quantum efficiency (EQE) of less than 10% at -10 V when the weight ratio of the two materials is 1 : 1 (wt/wt). The EQE of an OPD with P3HT:DRCN5T (100 : 2, wt/wt) as the active layer reaches 1400% at -10 V, exhibiting the photomultiplication (PM) phenomenon. The EQE values of PM-type OPDs can be markedly improved along with a bias increase, and the champion EQE reaches 10 600% at -20 V. The small number of small molecules can be used as electron traps due to the different lowest unoccupied molecular orbital (LUMO) levels of the two donors, and photogenerated electrons can be trapped in the small molecules surrounded by P3HT. The trapped electrons near the Al electrode can induce interfacial band bending for efficient hole tunneling injection from an external circuit. This work provides a new strategy for realizing acceptor-free PM-type OPDs, which may inspire us to further develop organic electronic devices with single type organic semiconducting materials.

Flexible Micropillar Electrode Arrays for In Vivo Neural Activity Recordings.

Flexible electronics that can form tight interfaces with neural tissues hold great promise for improving the diagnosis and treatment of neurological disorders and advancing brain/machine interfaces. Here, the facile fabrication of a novel flexible micropillar electrode array (µPEA) is described based on a biotemplate method. The flexible and compliant µPEA can readily integrate with the soft surface of a rat cerebral cortex. Moreover, the recording sites of the µPEA consist of protruding micropillars with nanoscale surface roughness that ensure tight interfacing and efficient electrical coupling with the nervous system. As a result, the flexible µPEA allows for in vivo multichannel recordings of epileptiform activity with a high signal-to-noise ratio of 252 ± 35. The ease of preparation, high flexibility, and biocompatibility make the µPEA an attractive tool for in vivo spatiotemporal mapping of neural activity.

Bacterial Cellulose as a Supersoft Neural Interfacing Substrate.

Biocompatible neural interfaces hold great promise for treating neurological disorders and enhancing the mental and physical ability of human beings. Most of the currently available neural interfaces are made from rigid, dense inorganic materials that cause tissue damage. We present supersoft multichannel electrodes by depositing gold layers on thin bacterial cellulose (BC) (Au-BC electrodes). The Young's modulus of BC ( EBC = 120 kPa) is between those of the brain tissue ( Ebrain = 2.7-3.1 kPa) and the peripheral neural tissues ( Eperipheral nerve = 580-840 kPa). The bending stiffness of the Au-BC electrodes corresponds to 1/5200 of Au-polyimide electrodes with the same layout. Furthermore, the Au-BC electrodes are highly durable (conductivity >95% after 100 cycles of 180° bending). In vivo recording of brain electric activity demonstrates the great potential of the Au-BC electrodes for neural interfacing applications.

Multiscale Hierarchical Design of a Flexible Piezoresistive Pressure Sensor with High Sensitivity and Wide Linearity Range.

Flexible piezoresistive pressure sensors have been attracting wide attention for applications in health monitoring and human-machine interfaces because of their simple device structure and easy-readout signals. For practical applications, flexible pressure sensors with both high sensitivity and wide linearity range are highly desirable. Herein, a simple and low-cost method for the fabrication of a flexible piezoresistive pressure sensor with a hierarchical structure over large areas is presented. The piezoresistive pressure sensor consists of arrays of microscale papillae with nanoscale roughness produced by replicating the lotus leaf's surface and spray-coating of graphene ink. Finite element analysis (FEA) shows that the hierarchical structure governs the deformation behavior and pressure distribution at the contact interface, leading to a quick and steady increase in contact area with loads. As a result, the piezoresistive pressure sensor demonstrates a high sensitivity of 1.2 kPa-1 and a wide linearity range from 0 to 25 kPa. The flexible pressure sensor is applied for sensitive monitoring of small vibrations, including wrist pulse and acoustic waves. Moreover, a piezoresistive pressure sensor array is fabricated for mapping the spatial distribution of pressure. These results highlight the potential applications of the flexible piezoresistive pressure sensor for health monitoring and electronic skin.

Simultaneous surface and depth neural activity recording with graphene transistor-based dual-modality probes.

Subdural surface and penetrating depth probes are widely applied to record neural activities from the cortical surface and intracortical locations of the brain, respectively. Simultaneous surface and depth neural activity recording is essential to understand the linkage between the two modalities. Here, we develop flexible dual-modality neural probes based on graphene transistors. The neural probes exhibit stable electrical performance even under 90° bending because of the excellent mechanical properties of graphene, and thus allow multi-site recording from the subdural surface of rat cortex. In addition, finite element analysis was carried out to investigate the mechanical interactions between probe and cortex tissue during intracortical implantation. Based on the simulation results, a sharp tip angle of π/6 was chosen to facilitate tissue penetration of the neural probes. Accordingly, the graphene transistor-based dual-modality neural probes have been successfully applied for simultaneous surface and depth recording of epileptiform activity of rat brain in vivo. Our results show that graphene transistor-based dual-modality neural probes can serve as a facile and versatile tool to study tempo-spatial patterns of neural activities.

Photomultiplication type narrowband organic photodetectors working at forward and reverse bias.

It is a great challenge to obtain narrowband and photomultiplication (PM) type organic photodetectors (OPDs) without optical filters due to the broad absorption range and large exciton binding energy of organic materials. Narrowband OPDs with the special structure of ITO/PFN-OX/P3HT : PC61BM (100 : 1,wt/wt)/Al were successfully fabricated with different active layer thicknesses, exhibiting a tunable response window and PM phenomenon under bi-directional bias. The OPDs exhibit U-shaped EQE spectra with two narrowband response windows under forward bias and a single narrowband response window under reverse bias. The best EQE of the optimized OPDs with a 4.0 µm thick active layer approaches 7160% or 8180% for 340 nm or 650 nm light illumination at 60 V and 1640% for 665 nm light illumination at -60 V, respectively. The most important features of the optimized OPDs is that the full width at half-maximum (FWHM) of their response windows is less than 30 nm under bi-directional biases, which can be well maintained at large bias. The PM type narrowband OPDs working at bi-directional bias are the first to be reported with a tunable response range, further indicating that the density of the electrons trapped in PC61BM near the hole injection electrode plays the key role in determining the interfacial band bending for hole tunneling injection from the external circuit.

Highly Narrowband Photomultiplication Type Organic Photodetectors.

Filterless narrowband response organic photodetectors (OPDs) present a great challenge due to the broad absorption range of organic semiconducting materials. The reported narrowband response OPDs also suffer from low external quantum efficiency (EQE) in the desired response window and low rejection ratio. Here, we report highly narrowband photomultiplication (PM) type OPDs based on P3HT:PC71BM (100:1, wt/wt) as active layer without an optical filter. The full width at half-maximum (fwhm) of the PM-type OPDs can be well retained less than 30 nm under different biases. Meanwhile, the champion EQE and rejection ratio approach 53 500% and 2020 at -60 V bias, respectively. The small fwhm should be attributed to the sharp absorption edge of active layer with small amount of PC71BM. The PM phenomenon is attributed to hole tunneling injection from the external circuit assisted by trapped electron in PC71BM near the Al electrode under light illumination. These highly narrowband PM-type OPDs should have great potential applications in sensitively detecting specific wavelength light and be blind to light outside of the desired response window.

Blown-Bubble Assembly and in Situ Fabrication of Sausage-like Graphene Nanotubes Containing Copper Nanoblocks.

We use a blown-bubble method to assemble Cu nanowires and in situ fabricate graphene-based one-dimensional heterostructures, including versatile sausage-like configurations consisting of multilayer graphene nanotubes (GNTs) filled by single or periodically arranged Cu nanoblocks (CuNBs). This is done by first assembling Cu nanowires among a polymer-based blown-bubble film (BBF) and then growing graphene onto the nanowire substrate using the polymer matrix as a solid carbon source by chemical-vapor deposition. The formation of sausage-like GNT@CuNB nanostructures is due to the partial melting and breaking of embedded Cu nanowires during graphene growth, which is uniquely related to our BBF process. We show that the GNT skin significantly slows the oxidation process of CuNBs compared with that of bare Cu nanowires, and the presence of stuffed CuNBs also reduces the linear resistance along the GNTs. The large-scale assembled graphene-based heterostructures achieved by our BBF method may have potential applications in heterojunction electronic devices and high-stability transparent conductive electrodes.

High Detectivity Graphene-Silicon Heterojunction Photodetector.

A graphene/n-type silicon (n-Si) heterojunction has been demonstrated to exhibit strong rectifying behavior and high photoresponsivity, which can be utilized for the development of high-performance photodetectors. However, graphene/n-Si heterojunction photodetectors reported previously suffer from relatively low specific detectivity due to large dark current. Here, by introducing a thin interfacial oxide layer, the dark current of graphene/n-Si heterojunction has been reduced by two orders of magnitude at zero bias. At room temperature, the graphene/n-Si photodetector with interfacial oxide exhibits a specific detectivity up to 5.77 × 10(13) cm Hz(1/2) W(-1) at the peak wavelength of 890 nm in vacuum, which is highest reported detectivity at room temperature for planar graphene/Si heterojunction photodetectors. In addition, the improved graphene/n-Si heterojunction photodetectors possess high responsivity of 0.73 A W(-1) and high photo-to-dark current ratio of ≈10(7) . The current noise spectral density of the graphene/n-Si photodetector has been characterized under ambient and vacuum conditions, which shows that the dark current can be further suppressed in vacuum. These results demonstrate that graphene/Si heterojunction with interfacial oxide is promising for the development of high detectivity photodetectors.