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Grain boundaries (GB) profoundly influence charge transport, and their localized potential barrier with a high density of defect states plays a crucial role in polycrystalline materials. There are a couple of models to estimate the density of states (DoS) of nanostructured materials in field-effect transistors (FETs) that probe interface traps between the semiconductor and dielectric but not at the grain boundaries. Here, we report on utilizing Levinson's and Seto's models of grain boundary transport and correlate them with the temperature-dependent hopping transport in copper iodide (CuI) polycrystalline nanoribbon (PNR) FETs. Experimentally, PNRs are obtained by e-beam lithography and thermal evaporation of CuI. To investigate the impact of GB, the devices are fabricated with different channel aspect ratios by varying widths (80, 260, and 570 nm) and lengths (20 to 90 µm). Owing to the high hole concentration, PNR FETs operate in depletion mode at 300 K. At various low temperatures (80-300 K), the figures-of-merits of FETs are estimated to understand device performance. We determine GB barrier heights, activation energy, and density of GB trap states and find equivalence between the two models. Furthermore, we calculate temperature-dependent hopping and trap-limited transport parameters to obtain DoS at the Fermi energy, trapped and free charge carrier density, localization length, hopping distance, hopping energy, etc. at various channel lengths. Based on this quantitative analysis, we propose a channel length-dependent GB barrier height variation due to the in-plane electric field and elucidate CuI energy band levels.
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Flat panel reactors, coated with photocatalytic materials, offer a sustainable approach for the commercial production of hydrogen (H2) with zero carbon footprint. Despite this, achieving high solar-to-hydrogen (STH) conversion efficiency with these reactors is still a significant challenge due to the low utilization efficiency of solar light and rapid charge recombination. Herein, hybrid gold nano-islands (HGNIs) are developed on transparent glass support to improve the STH efficiency. Plasmonic HGNIs are grown on an in-house developed active glass sheet composed of sodium aluminum phosphosilicate oxide glass (H-glass) using the thermal dewetting method at 550 °C under an ambient atmosphere. HGNIs with various oxidation states (Au0, Au+, and Au-) and multiple interfaces are obtained due to the diffusion of the elements from the glass structure, which also facilitates the lifetime of the hot electron to be ≈2.94 ps. H-glass-supported HGNIs demonstrate significant STH conversion efficiency of 0.6%, without any sacrificial agents, via water dissociation. This study unveils the specific role of H-glass-supported HGNIs in facilitating light-driven chemical conversions, offering new avenues for the development of high-performance photocatalysts in various chemical conversion reactions for large-scale commercial applications.
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In the contemporary way of life, face masks are crucial in managing disease transmission and battling air pollution. However, two key challenges, self-sanitization and biodegradation of face masks, need immediate attention, prompting the development of innovative solutions for the future. In this study, we present a novel approach that combines controlled acid hydrolysis and mechanical chopping to synthesize a silk nanofibrous network (SNN) seamlessly integrated with a wearable stainless steel mesh, resulting in the fabrication of self-sanitizable face masks. The distinct architecture of face masks showcases remarkable filtration efficiencies of 91.4, 95.4, and 98.3% for PM0.3, PM0.5, and PM1.0, respectively, while maintaining a comfortable level of breathability (ΔP = 92 Pa). Additionally, the face mask shows that a remarkable thermal resistance of 472 °C cm2 W-1 generates heat spontaneously at low voltage, deactivating Escherichia coli bacteria on the SNN, enabling self-sanitization. The SNN exhibited complete disintegration within the environment in just 10 days, highlighting the remarkable biodegradability of the face mask. The unique advantage of self-sanitization and biodegradation in a face mask filter is simultaneously achieved for the first time, which will open avenues to accomplish environmentally benign next-generation face masks.
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Two-dimensional (2D) transition-metal carbides (MXenes) are emerging as promising materials for a wide range of applications owing to their intriguing electrical, optical, and optoelectronic properties. However, the modulation of metallic Ti3C2Tx MXene electronic properties is the key challenge to fabricate functional nanoelectronic devices. Here, we demonstrate a solution-processable route to fabricate Ti3C2Tx MXene/CuI nanoparticle heterointerfaces by employing a layer-by-layer assembly process. The charge transfer at the heterointerfacial assembly is monitored qualitatively from the quenched photoluminescence emission of CuI. The stable electrical conductivity and consistent Raman spectra of the 3-LBL assembly (three sequential stacks of CuI/MXene) signify the oxidation stability of Ti3C2Tx thin films even after exposure to the ambient environment for 2 months. Furthermore, the 3-LBL assembly exhibited a three-dimensional (3D) variable-range hopping-based electrical conduction in the temperature range 2 ≤ T < 100 K, contrary to the weak localized transport phenomenon in Ti3C2Tx MXene. The difference in charge transport mechanism is supported by distinct magnetoresistance (MR) of the Ti3C2Tx MXene (negative MR, -0.4%) and 3-LBL assembly (positive MR, 1.6%). Therefore, the modulated electrical transport and superior oxidation stability of the Ti3C2Tx MXene in the 3-LBL assembly have the potential to develop next-generation optoelectronic and memory devices.
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The emergence of organic-inorganic hybrid perovskites (OHPs) has revolutionised the potential performance of optoelectronic devices; most perovskites are opaque and hence incompatible with transparent optoelectronics and sensitive to environmental degradation. Here, we have reported a single-step fabrication of ultra-long MAPbI3 perovskite microwire arrays over a large area using stencil lithography based on sequential vacuum sublimation. The environmental stability of MAPbI3 is empowered with a newly designed and synthesized transparent supramolecular self-assembly based on a mixture of two tripodal l-Phe-C11H23/C7F15 molecules, which showed a contact angle of 105° and served as ultra-hydrophobic passivation layers for more than 45 days in an ambient atmosphere. The MAPbI3 microwire arrays passivated with the supramolecular self-assembly demonstrated for the first time both excellent transparency of â¼89% at 550 nm and a remarkable photoresponse with a photo-switching ratio of â¼104, responsivity of 789 A W-1, detectivity of 1014 Jones, linear dynamic range of â¼122 dB, and rise time of 432 µs. Furthermore, the photodetector fabricated on a flexible PET substrate demonstrated robust mechanical flexibility even beyond 1200 bending cycles. Therefore, the scalable stencil lithography and supramolecular passivation approaches have the potential to deliver next-generation transparent, flexible, and stable optoelectronic devices.
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Unveiling the transparency and flexibility in perovskite-based photodetectors with superior photoresponse and environmental stability remains an open challenge. Here we report on guanidinium incorporated metal halide perovskite (MA1-xGuaxPbI3, x = 0 to 0.65) random percolative microstructure (RPM) fabrication using an ultra-fast spray coating technique. Remarkably, RPMs over a large area of 5 × 5 cm2 on flexible substrates with a transparency of â¼50% can be achieved with enriched environmental stability. Transparent photodetectors based on MA1-xGuaxPbI3 (x = 0.12) RPMs manifest excellent performance with a responsivity of 187 A W-1, a detectivity of 2.23 × 1012 Jones and an external quantum efficiency of 44 115%. Additionally, the photodetectors exhibited superior mechanical flexibility under a wide range of bending angles and large number of binding cycles. Integrating features including transparency, high performance, stability, flexibility and scalability within a photodetector is unmatched and holds potential for novel applications in transparent and wearable optoelectronic devices.
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Desiccation of a colloidal layer produces crack patterns because of stress arising out of solvent evaporation. Associated with it is the rearrangement of particles, while adhesion to the substrate resists such movements. The nature of solvent, which is often overlooked, plays a key role in the process as it dictates evaporation and wetting properties of the colloidal film. Herein, we study the crack formation process by using a mixture of solvents, water, and isopropyl alcohol (IPA). Among the various ratios, a water/IPA mixture (15:85 by volume) close to the azeotropic composition possesses unusual evaporation and wetting properties, leading to narrower cracks with widths down to â¼162 nm, uncommon among the known crackle patterns. The dense and narrow crack patterns have been used as sacrificial templates to obtain metal meshes on transparent substrates for optoelectronic applications.
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Monitoring live movements of human body parts is becoming increasingly important in the context of biomedical and human machine technologies. The development of wearable strain sensors with high sensitivity and fast response is critical to address this need. In this article, we describe the fabrication of a wearable strain sensor made of a Au micromesh partially embedded in polydimethylsiloxane substrate. The sensor exhibits a high optical transmittance of 85%. The effective strain range for stretching is 0.02%-4.5% for a gauge factor of over 108. In situ scanning electron imaging and infrared thermal microscopy analysis have revealed that nanometric break junctions form throughout the wire network under strain; strain increases the number of such junctions, leading to a large change in the sheet resistance of the mesh. This aspect has been examined computationally with the findings that wire segments break successively with increasing strain and resistance increases linearly for lower values of strain and nonlinearly at higher values of strain because of formation of current bottlenecks. The semi-embedded nature of these Au microwires allows the broken wires to retract to the original positions, thus closing the nanogaps and regaining the original low resistance state. High repeatability as well as cyclic stability have been demonstrated in live examples involving human body activity, importantly while mounting the sensor in strategic remote locations away from the most active site where strains are highest.
Asunto(s)
Cara , Masticación , Movimiento , Dispositivos Electrónicos Vestibles , HumanosRESUMEN
Optically transparent photodetectors are crucial in next-generation optoelectronic applications including smart windows and transparent image sensors. Designing photodetectors with high transparency, photoresponsivity, and robust mechanical flexibility remains a significant challenge, as is managing the inevitable trade-off between high transparency and strong photoresponse. Here we report a scalable method to produce flexible crystalline Si nanostructured wire (NW) networks fabricated from silicon-on-insulator (SOI) with seamless junctions and highly responsive porous Si segments that combine to deliver exceptional performance. These networks show high transparency (â¼92% at 550 nm), broadband photodetection (350 to 950 nm) with excellent responsivity (25 A/W), optical response time (0.58 ms), and mechanical flexibility (1000 cycles). Temperature-dependent photocurrent measurements indicate the presence of localized electronic states in the porous Si segments, which play a crucial role in light harvesting and photocarrier generation. The scalable low-cost approach based on SOI has the potential to deliver new classes of flexible optoelectronic devices, including next-generation photodetectors and solar cells.
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Despite relatively high manufacturing cost, crystalline-Si solar cell continues to hold promising future due to its high energy conversion efficiency and long life. As regards cost, one pertinent issue is the top electrode metallization of textured cell surface, which typically involves screen printing of silver paste. The associated disadvantages call for alternative methods that can lower the cost without compromising the solar cell efficiency. In the present work, a highly interconnected one-dimensional (1D) metal wire network has been employed as front electrode on conventional Si wafers. Here, for the first time, we report an innovative solution based crackle templating method for conformal metal wire network patterning over large textured surfaces. Laser beam induced current mapping showed uniform photocurrent collection by the electrodes without any shadow losses. With electroless deposition of Ni wire network on corrugated solar cell, a short circuit current of 33.28 mA/cm2 was obtained in comparison to 20.53 mA/cm2 without the network electrode. On comparing the efficiency with the conventional cells with screen printed electrodes, a 20% increment in efficiency has been observed. Importantly, the estimated manufacturing cost is at least two orders lower.
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A high degree of transparency in devices is considered highly desirable for futuristic technology. This demands that both the active material and the electrodes are made of transparent materials. In this work, a transparent Pd wire network (â¼1 cm(2)), fabricated using crackle lithography technique with sheet resistance and transmittance of â¼200 Ohm per square and â¼80%, respectively, serves multiple roles; besides being an electrode, it acts as an active material for H2 sensing as well as an in-built electrothermal heater. The sensor works over a wide range of hydrogen (H2) concentration down to 0.02% with a response time of â¼41 s, which could be improved to â¼13 s by in situ Joule heating to â¼75 °C. Importantly, the device has the potential of scale-up to a window size transparent panel and to be flexible when desired.
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Heater plates or sheets that are visibly transparent have many interesting applications in optoelectronic devices such as displays, as well as in defrosting, defogging, gas sensing and point-of-care disposable devices. In recent years, there have been many advances in this area with the advent of next generation transparent conducting electrodes (TCE) based on a wide range of materials such as oxide nanoparticles, CNTs, graphene, metal nanowires, metal meshes and their hybrids. The challenge has been to obtain uniform and stable temperature distribution over large areas, fast heating and cooling rates at low enough input power yet not sacrificing the visible transmittance. This review provides topical coverage of this important research field paying due attention to all the issues mentioned above.
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Transparent conducting electrodes (TCEs) have been made on flat, flexible, and curved surfaces, following a crack template method in which a desired surface was uniformly spray-coated with a crackle precursor (CP) and metal (Ag) was deposited by vacuum evaporation. An acrylic resin (CP1) and a SiO2 nanoparticle-based dispersion (CP2) derived from commercial products served as CPs to produce U-shaped cracks in highly interconnected networks. The crack width and the density could be controlled by varying the spray conditions, resulting in varying template thicknesses. By depositing Ag in the crack regions of the templates, we have successfully produced Ag wire network TCEs on flat-flexible PET sheets, cylindrical glass tube, flask and lens surface with transmittance up to 86%, sheet resistance below 11 Ω/â¡ for electrothermal application. When used as a transparent heater by joule heating of the Ag network, AgCP1 and AgCP2 on PET showed high thermal resistance values of 515 and 409 °C cm(2)/W, respectively, with fast response (<20 s), requiring only low voltages (<5 V) to achieve uniform temperatures of â¼100 °C across large areas. Similar was the performance of the transparent heater on curved glass surfaces. Spray coating in the context of crack template is a powerful method for producing transparent heaters, which is shown for the first time in this work. AgCP1 with an invisible wire network is suited for use in proximity while AgCP2 wire network is ideal for use in large area displays viewed from a distance. Both exhibited excellent defrosting performance, even at cryogenic temperatures.
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We report a highly transparent, low resistance Ag metal network templated by a cracked polymer thin film and its incorporation in an organic solar cell. The performance of this scalable metallic network is comparable to that of conventional ITO electrodes. This is a general approach to replace ITO in diverse thin film devices.
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A transparent conductor which can generate high temperatures finds important applications in optoelectronics. In this article, a wire network made of Au on quartz is shown to serve as an effective high temperature transparent heater. The heater has been fabricated by depositing Au onto a cracked sacrificial template. The highly interconnected Au wire network thus formed exhibited a transmittance of â¼87% in a wide spectral range with a sheet resistance of 5.4 Ω â¡(-1). By passing current through the network, it could be joule heated to â¼600 °C within a few seconds. The extraordinary thermal performance and stability owe much to the seamless junctions present in the wire network. Furthermore, the wire network gets self-annealed through joule heating as seen from its increased crystallinity. Interestingly, both transmittance and sheet resistance improved following annealing to 92% and 3.2 Ω â¡(-1), respectively.
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We report a simple lithography-free, solution-based method of soldering of carbon nanotubes with Ohmic contacts, by taking specific examples of multi-walled carbon nanotubes (MWNTs). This is achieved by self-assembling a monolayer of soldering precursor, Pd(2+) anchored to 1,10 decanedithiol, onto which MWNTs could be aligned across the gap electrodes via solvent evaporation. The nanosoldering was realized by thermal/electrical activation or by both in sequence. Electrical activation and the following step of washing ensure selective retention of MWNTs spanning across the gap electrodes. The soldered joints were robust enough to sustain strain caused during the bending of flexible substrates as well as during ultrasonication. The estimated temperature generated at the MWNT-Au interface using an electro-thermal model is â¼150 °C, suggesting Joule heating as the primary mechanism of electrical activation. Further, the specific contact resistance is estimated from the transmission line model.