Photo-Enhanced Chemo-Transistor Platform for Ultrasensitive Assay of Small Molecules.

Compared with traditional assay techniques, field-effect transistors (FETs) have advantages such as fast response, high sensitivity, being label-free, and point-of-care detection, while lacking generality to detect a wide range of small molecules since most of them are electrically neutral with a weak doping effect. Here, we demonstrate a photo-enhanced chemo-transistor platform based on a synergistic photo-chemical gating effect in order to overcome the aforementioned limitation. Under light irradiation, accumulated photoelectrons generated from covalent organic frameworks offer a photo-gating modulation, amplifying the response to small molecule adsorption including methylglyoxal, p-nitroaniline, nitrobenzene, aniline, and glyoxal when measuring the photocurrent. We perform testing in buffer, artificial urine, sweat, saliva, and diabetic mouse serum. The limit of detection is down to 10-19 M methylglyoxal, about 5 orders of magnitude lower than existing assay technologies. This work develops a photo-enhanced FET platform to detect small molecules or other neutral species with enhanced sensitivity for applications in fields such as biochemical research, health monitoring, and disease diagnosis.

Self-Expanding Molten Salt-Driven Growth of Patterned Transition-Metal Dichalcogenide Crystals.

Transition-metal dichalcogenides (TMDs) have been considered potential materials for the next generation of semiconductors. Realizing controllable growth of TMD crystals is a prerequisite for their future applications, which remains challenging. Here, we reveal a new mechanism of self-expanding molten salt-driven growth for a salt-assisted method and achieve the patterned growth of TMD single-crystal arrays with a size of hundreds of micrometers. Time-of-flight secondary ion mass spectroscopy and other spectroscopy characterizations identify the component of the molten salt solution. Microscopic characterizations reveal the existence of salt solution as an interlayer between a TMD monolayer and the silicon substrate as well as particles along the crystal edge. The edged salt solution serves as a self-expanding liquid substrate, which confines the reactive sites to the localized liquid surface, thus avoiding random nucleation. The surface reaction also assures monolayer crystal formation due to self-limiting growth. Besides, the liquid substrate affords sources and spreads itself continuously owing to the nonwetting effect on TMD crystals, thereby facilitating the continuous extension of the TMD monolayer. This work provides novel insights into the controllable synthesis of TMD monolayers and paves the way for the fabrication of TMD-based integrated functional devices.

Ultrasensitive Detection of SARS-CoV-2 Antibody by Graphene Field-Effect Transistors.

The fast spread of SARS-CoV-2 has severely threatened the public health. Establishing a sensitive method for SARS-CoV-2 detection is of great significance to contain the worldwide pandemic. Here, we develop a graphene field-effect transistor (g-FET) biosensor and realize ultrasensitive SARS-CoV-2 antibody detection with a limit of detection (LoD) down to 10-18 M (equivalent to 10-16 g mL-1) level. The g-FETs are modified with spike S1 proteins, and the SARS-CoV-2 antibody biorecognition events occur in the vicinity of the graphene surface, yielding an LoD of ∼150 antibodies in 100 µL full serum, which is the lowest LoD value of antibody detection. The diagnoses time is down to 2 min for detecting clinical serum samples. As such, the g-FETs leverage rapid and precise SARS-CoV-2 screening and also hold great promise in prevention and control of other epidemic outbreaks in the future.

Excimer Ultraviolet-Irradiated Carbon Nanofibers as Advanced Anodes for Long Cycle Life Lithium-Ion Batteries.

Carbon nanofibers (CNFs) bearing oxygen-containing functional groups and inhomogeneous nanopores are successfully prepared by excimer UV radiation. The CNFs demonstrate potential for use as an anodic material in rechargeable Li-ion batteries. Their improved electrochemical performances are attributed to the chemically bonded solid-electrolyte interface films on the CNF surface. This approach is also applicable to other carbonaceous electrode materials.

Photovoltaic nanocells for high-performance large-scale-integrated organic phototransistors.

A high-performance large-scale-integrated organic phototransistor needs a semiconductor layer that maintains its photoelectric conversion ability well during high-resolution pixelization. However, lacking a precise design for the nanoscale structure, a trade-off between photoelectric performance and device miniaturization greatly limits the success in commercial application. Here we demonstrate a photovoltaic-nanocell enhancement strategy, which overcomes the trade-off and enables high-performance organic phototransistors at a level beyond large-scale integration. Embedding a core-shell photovoltaic nanocell based on perovskite quantum dots in a photocrosslinkable organic semiconductor, ultralarge-scale-integrated (>221 units) imaging chips are manufactured using photolithography. 27 million pixels are interconnected and the pixel density is 3.1 × 106 units cm-2, at least two orders of magnitude higher than in existing organic imaging chips and equivalent to the latest commercial full-frame complementary metal-oxide-semiconductor camera chips. The embedded photovoltaic nanocells induce an in situ photogating modulation and enable photoresponsivity and detectivity of 6.8 × 106 A W-1 and 1.1 × 1013 Jones (at 1 Hz), respectively, achieving the highest values of organic imaging chips at large-scale or higher integration. In addition, a very-large-scale-integrated (>216 units) stretchable biomimetic retina based on photovoltaic nanocells is manufactured for neuromorphic imaging recognition with not only resolution but also photoresponsivity and power consumption approaching those of the biological counterpart.

Patterning an Erosion-Free Polymeric Semiconductor Channel for Reliable All-Photolithography Organic Electronics.

Reliable patterning of organic semiconductors (OSCs) with high uniformity is essential to all-photolithography organic electronics. However, the majority of cross-linked OSCs experience performance fluctuations after photolithography because of the inherent vulnerability of low-ordered regions. Herein, we develop an anti-solution penetration photolithography process to achieve the reliable patterning of the OSC layer for all-photolithography integrated organic electronics. Using a thick and highly cross-linked semiconductor film and a low-solubility developer, an erosion-free semiconductor channel is obtained with a high mobility of up to 1.254 cm2 V-1 s-1 and a uniform threshold voltage close to zero. Compared with existing all-photolithography organic circuits, the unit logic gate area consumption is lower by 1-3 orders of magnitude at 0.0069 mm2, while the transistor density is higher by 1-2 orders of magnitude at 6780 Tr cm-2. The miniaturized organic inverters maintain uncompromised voltage gains, and the 15-stage organic ring oscillators feature higher oscillation frequencies, making them promising for applications in wide-ranging integrated organic circuits.

A comprehensive nano-interpenetrating semiconducting photoresist toward all-photolithography organic electronics.

Owing to high resolution, reliability, and industrial compatibility, all-photolithography is a promising strategy for industrial manufacture of organic electronics. However, it receives limited success due to the absence of a semiconducting photoresist with high patterning resolution, mobility, and performance stability against photolithography solution processes. Here, we develop a comprehensive semiconducting photoresist with nano-interpenetrating structure. After photolithography, nanostructured cross-linking networks interpenetrate with continuous phases of semiconducting polymers, enabling submicrometer patterning accuracy and compact molecular stacking with high thermodynamic stability. The mobility reaches the highest values of photocrosslinkable organic semiconductors and maintains almost 100% after soaking in developer and stripper for 1000 min. Owing to the comprehensive performance, all-photolithography is achieved, which fabricates organic inverters and high-density transistor arrays with densities up to 1.1 × 105 units cm-2 and 1 to 4 orders larger than conventional printing processes, opening up a new approach toward manufacturing highly integrated organic circuits and systems.

[Inhibition of Jingzhaotoxin-V on Kv4.3 channel].

Kv4.3 channel is present in many mammalian tissues, predominantly in the heart and central nervous system. Its currents are transient, characterized by rapid activation and inactivation. In the hearts of most mammals, it is responsible for repolarization of the action potential of ventricular myocytes and is important in the regulation of the heart rate. Because of its central role in this important physiological process, Kv4.3 channel is a promising target for anti-arrhythmic drug development. Jingzhaotoxin-V (JZTX-V) is a novel peptide neurotoxin isolated from the venom of the spider Chilobrachys jingzhao. Whole-cell patch clamp recording showed that it partly blocked the transient outward potassium channels in dorsal root ganglion neurons of adult rats with an IC(50) value of 52.3 nmol/L. To investigate the effect of JZTX-V on Kv4.3 channel, JZTX-V was synthesized using the solid-phase chemical synthesis and separated by reverse phase high performance liquid chromatography (HPLC). The purity was tested by matrix-assisted laser desorption-ionization time-of-flight mass spectrometry (MOLDI-TOF mass spectrometry). Two-electrode voltage-clamp technique was used to characterize the action of JZTX-V on Kv4.3 channels expressed in Xenopus laevis oocytes. As a result, JZTX-V displayed fast kinetics of inhibition and recovery from inactivation. Furthermore, it could inhibit Kv4.3 channel current in a time- and concentration-dependent manner with an IC(50) value of 425.1 nmol/L. The application of JZTX-V affected the activation and inactivation characteristics of Kv4.3 channel and caused a shift of the current-voltage relationship curve and the steady-state inactivation curve to depolarizing direction by approximately 29 mV and 10 mV, respectively. So we deduced that JZTX-V is a gating modifier toxin of Kv4.3 channel. Present findings should be helpful to develop JZTX-V into a molecular probe and drug candidate targeting to Kv4.3 channel in the myocardium.

Excimer ultraviolet-irradiated exfoliated graphite loaded with carbon-coated SnOx small nanoparticles as advanced anodes for high-rate-capacity lithium-ion batteries.

This paper reports a fast and efficient excimer ultraviolet (EUV) radiation method to prepare carbon-coated mixed tin oxide-loaded exfoliated graphite (SnOx@C-G) nanocomposites. The SnOx small nanoparticles (SNPs) are isolated using oxidized sucrose and uniformly deposited onto mildly oxidized exfoliated graphite during the 20-minute EUV radiation process. XPS and ESR analyses suggest the existence of abundant oxygen vacancies in the SnOx SNPs. The electrochemical kinetics of SnOx@C-G, which are determined by in situ electrochemical impedance analysis, demonstrated a high reversible capacity of approximately 740 mA h g-1 after 250 cycles at a current density of 1.6 A g-1, and an impressive reversible rate performance exceeding 450 mA h g-1 can be obtained even at a high current density of 3.2 A g-1 when applied as an anode for lithium storage. This improved cycling stability and rate capability benefit from the carbon coating, which not only buffers the volume change of SnOx SNPs but also provides a path for electron transport on the surface of the SnOx SNPs during the electrochemical process. Furthermore, the oxygen vacancies in SnOx SNPs result in a large capacitive contribution to capacity. The EUV radiation method used to synthesize SnOx@C-graphite nanosheets is universally applicable to prepare a high-performance SNPs/carbon-based anode for lithium-ion batteries.

Controlled Synthesis of Carbon Nanofibers Anchored with Zn(x)Co(3-x)O4 Nanocubes as Binder-Free Anode Materials for Lithium-Ion Batteries.

The direct growth of complex ternary metal oxides on three-dimensional conductive substrates is highly desirable for improving the electrochemical performance of lithium-ion batteries (LIBs). We herein report a facile and scalable strategy for the preparation of carbon nanofibers (CNFs) anchored with ZnxCo3-xO4 (ZCO) nanocubes, involving a hydrothermal process and thermal treatment. Moreover, the size of the ZCO nanocubes was adjusted by the quantity of urea used in the hydrothermal process. Serving as a binder-free anode material for LIBs, the ZnCo2O4/CNFs composite prepared using 1.0 mmol of urea (ZCO/CNFs-10) exhibited excellent electrochemical performance with high reversible capacity, excellent cycling stability, and good rate capability. More specifically, a high reversible capacity of ∼600 mAh g(-1) was obtained at a current density of 0.5 C following 300 charge-discharge cycles. The excellent electrochemical performance could be associated with the controllable size of the ZCO nanocubes and synergistic effects between ZCO and the CNFs.