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Sonochemical decomposition effects of nickelocene, which sublimates easily were investigated to synthesize dispersant-free nickel fine particles at low temperature. In a hydrazine monohydrate and 2-propanol mixed solvent, the reduction of nickelocene was promoted by ultrasound irradiation, and nickel fine particles were synthesized while precluding the sublimation of nickelocene. Unlike the common hydrazine reduction of nickel salts, which requires multiple-step reactions, nickelocene was reduced directly without forming intermediates. The effect of the water-bath temperature (20-60 °C) was investigated, where larger fine particles were synthesized using a higher water-bath temperature (60 °C). When irradiated at 20 °C, the reduction rate of nickelocene was low, leading to the formation of nickel fine particles and organic nanoparticles via the reduction and decomposition of nickelocene. The ultrasound frequency was also investigated, where fine nickel particles were synthesized using low-frequency ultrasound irradiation. The formation of high-temperature hotspots led to the diffusion and growth of nickel on the surface of the nickel fine particles; therefore, raspberry-like nickel fine particles were synthesized. In this study, the difficult-to-handle nature of nickelocene, owing to its sublimation properties, was easily overcome by ultrasound irradiation. Instantaneous and localized reactions at hotspots contributed to inhibiting particle growth. Furthermore, Ni fine particles were synthesized via a direct reduction pathway, which differs from previous reactions. This method represents a new, dispersant-free, low-temperature process for synthesizing Ni fine particles.

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A novel approach to fabricating a transparent and flexible one-transistor-one-diode (1T-1D) image sensor array on a flexible colorless polyimide (CPI) film substrate is successfully demonstrated with laser lift-off (LLO) techniques. Leveraging transparent indium tin oxide (ITO) electrodes and amorphous indium gallium zinc oxide (a-IGZO) channel-based thin-film transistor (TFT) backplanes, vertically stacked p-i-n hydrogenated amorphous silicon (a-Si:H) photodiodes (PDs) utilizing a low-temperature (<90 °C) deposition process are integrated with a densely packed 14 × 14 pixel array. The low-temperature-processed a-Si:H photodiodes show reasonable performance with responsivity and detectivity for 31.43 mA/W and 3.0 × 1010 Jones (biased at -1 V) at a wavelength of 470 nm, respectively. The good mechanical durability and robustness of the flexible image sensor arrays enable them to be attached to a curved surface with bending radii of 20, 15, 10, and 5 mm and 1000 bending cycles, respectively. These studies show the significant promise of utilizing highly flexible and rollable active-matrix technology for the purpose of dynamically sensing optical signals in spatial applications.

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Improving the mechanical strength of ceramic solid electrolytes such as lithium phosphorus sulfide families for pressure-driven dendrite blocking as well as reducing the electronic conductivity to prevent a dendrite formation inside the electrolytes are very important to extend the lifespan of all-solid-state lithium-metal batteries. Here, we propose a low-temperature solution-precipitation process to prepare polymer-solid electrolyte composites for a highly uniform polymer distribution in the electrolyte to enhance their mechanical strength and reduce their electronic conduction. The composites with up to 12 wt % of polymer are prepared, and the composites exhibit high ionic conductivities of up to 0.3 mS/cm. Furthermore, the electrochemical stability of the electrolyte composites on Li striping/plating cycles is investigated. We confirm that the proposed solution-precipitation process makes the composite much more stable than the bare solid electrolyte and causes them to outperform similar composites from the other existing preparation methods, such as mechanical mixing and solution dispersion.

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In recent printed electronics technology, a photo-sintering technique using intense pulsed light (IPL) source has attracted attention, instead of conventional a thermal sintering process with long time and high temperature. The key principle of the photo-sintering process is the selective heating of a thin film with large light absorption coefficients, while a transparent substrate does not heat by the IPL source. Most research on photo-sintering has used a xenon flash lamp as a light source. However, the xenon flash lamp requires instantaneous high power and is unsuitable for large area applications. In this work, we developed a new photo-sintering system using a high-power ultraviolet light emitting diode (UV-LED) module. A LED light source has many merits such as low power consumption and potential large-scale application. The silver nanoparticles ink was inkjet-printed on a polyethylene terephthalate (PET) and photo-sintered by the UV-LED module with the wavelength of 365 and 385 nm. The electrical resistivity as low as 5.44 × 10-6 Ω·cm (just about three times compared to value of bulk silver) was achieved at optimized photo-sintering conditions (wavelength of 365 nm and light intensity of 300 mW/cm2).

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This study reports a strong ME effect in thin-film composites consisting of nickel, iron, or cobalt foils and 550 nm thick AlN films grown by PE-ALD at a (low) temperature of 250 °C and ensuring isotropic and highly conformal coating profiles. The AlN film quality and the interface between the film and the foils are meticulously investigated by means of high-resolution transmission electron microscopy and the adhesion test. An interface (transition) layer of partially amorphous AlxOy/AlOxNy with thicknesses of 10 and 20 nm, corresponding to the films grown on Ni, Fe, and Co foils, is revealed. The AlN film is found to be composed of a mixture of amorphous and nanocrystalline grains at the interface. However, its crystallinity is improved as the film grew and shows a highly preferred (002) orientation. High self-biased ME coefficients (αME at a zero-bias magnetic field) of 3.3, 2.7, and 3.1 V·cm-1·Oe-1 are achieved at an off-resonance frequency of 46 Hz in AlN/Ni thin-film composites with different Ni foil thicknesses of 7.5, 15, and 30 µm, respectively. In addition, magnetoelectric measurements have also been carried out in composites made of 550 nm thick films grown on 12.5 µm thick Fe and 15 µm thick Co foils. The maximum magnetoelectric coefficients of AlN/Fe and AlN/Co composites are 0.32 and 0.12 V·cm-1·Oe-1, measured at 46 Hz at a bias magnetic field (Hdc) of 6 and 200 Oe, respectively. The difference of magnetoelectric transducing responses of each composite is discussed according to interface analysis. We report a maximum delivered power density of 75 nW/cm3 for the AlN/Ni composite with a load resistance of 200 kΩ to address potential energy harvesting and electromagnetic sensor applications.

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Highly customized and free-formed products in flexible hybrid electronics (FHE) require direct pattern creation such as inkjet printing (IJP) to accelerate product development. In this work, we demonstrate the direct growth of graphene on Cu ink deposited on polyimide (PI) by means of plasma-enhanced chemical vapor deposition (PECVD), which provides simultaneous reduction, sintering, and passivation of the Cu ink and further reduces its resistivity. We investigate the PECVD growth conditions for optimizing the graphene quality on Cu ink and find that the defect characteristics of graphene are sensitive to the H2/CH4 ratio at higher total gas pressure during the growth. The morphology of Cu ink after the PECVD process and the dependence of the graphene quality on the H2/CH4 ratio may be attributed to the difference in the corresponding electron temperature. Therefore, this study paves a new pathway toward efficient growth of high-quality graphene on Cu ink for applications in flexible electronics and Internet of Things (IoT).

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The dynamic tuning of ion concentrations has attracted significant attention for creating versatile functionalities of materials, which are impossible to reach using classical control knobs. Despite these merits, the following fundamental questions remain: how do ions affect the electronic bandstructure, and how do ions simultaneously change the electrical and magnetic properties? Here, by annealing platinum-dotted La0.67 Sr0.33 MnO3 films in hydrogen and argon at a lower temperature of 200 °C for several minutes, a reversible change in resistivity is achieved by three orders of magnitude with tailored ferromagnetic magnetization. The transition occurs through the tuning of the double exchange interaction, ascribed to an electron-doping-induced and/or a lattice-expansion-induced modulation, along with an increase in the hydrogen concentration. High reproducibility, long-term stability, and multilevel linearity are appealing for ionic-electric-magnetic coupled applications.

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Oil-in-water nanoemulsions are used in numerous biomedical applications as delivery systems. The droplet size in the nanometer range and their composition were extensively developed for carrying and enhancing the absorption of lipophilic drugs and lipids of interest. In the present study, critical parameters involved in the spontaneous nanoemulsification process such as the temperature, the oil type, the surfactant-to-oil and water-to-oil ratios were investigated. The aim was to design a solvent-free procedure for the spontaneous nanoemulsification at a low temperature of a large variety of triglycerides including vegetable oils. Nanoemulsification of medium-chain triglyceride (MCT) was not dependent on the temperature while nanodroplets of long-chain triglycerides (LCT) were only obtained by reaching the cloud point of ethoxylated surfactant Kolliphor® HS15. The molar volume of triglycerides was considered as a predictive parameter governing both, the spontaneous nanoemulsification at low temperature and the Ostwald ripening rate. The physical mixture of MCT and LCT was a promising strategy to prepare stable and fine nanoemulsions at 37 °C. They were characterized by a hydrodynamic diameter comprised between 20 and 30 nm and a narrow size distribution. These findings pave the way to new applications for the parenteral nutrition and the delivery of thermosensitive drugs and lipophilic molecules such as antioxidants.

Asunto(s)

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The development of novel dielectric materials with reliable dielectric properties and low-temperature processibility is crucial to manufacturing flexible and high-performance organic thin-film transistors (OTFTs) for next-generation roll-to-roll organic electronics. Here, we investigate the solution-based fabrication of high-k aluminum oxide (Al2O3) thin films for high-performance OTFTs. Nanocluster-based Al2O3 films fabricated by highly energetic photochemical activation, which allows low-temperature processing, are compared to the conventional nitrate-based Al2O3 films. A wide array of spectroscopic and surface analyses show that ultralow-temperature photochemical activation (<60 °C) induces the decomposition of chemical impurities and causes the densification of the metal-oxide film, resulting in a highly dense high-k Al2O3 dielectric layer from Al-13 nanocluster-based solutions. The fabricated nanocluster-based Al2O3 films exhibit a low leakage current density (<10-7 A/cm2) at 2 MV/cm and high dielectric breakdown strength (>6 MV/cm). Using this dielectric layer, precisely aligned microrod-shaped 2,7-dioctyl[1]benzothieno [3,2-b][1] benzothiophene (C8-BTBT) single-crystal OTFTs were fabricated via solvent vapor annealing and photochemical patterning of the sacrificial layer.

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High-performance In-Ga-Zn-O (IGZO) Schottky diodes (SDs) were fabricated using hydrogenated IGZO (IGZO:H) at a maximum process temperature of 150 °C. IGZO:H was prepared by Ar + O2 + H2 sputtering. IGZO:H SDs on a glass substrate exhibited superior electrical properties with a very high rectification ratio of 3.8 × 1010, an extremely large Schottky barrier height of 1.17 eV, and a low ideality factor of 1.07. It was confirmed that the hydrogen incorporated during IGZO:H deposition increased the band gap energy from 3.02 eV (IGZO) to 3.29 eV (IGZO:H). Thus, it was considered that the increase in band gap energy (decrease in electron affinity) of IGZO:H contributed to the increase in the Schottky barrier height of the SDs. Angle-resolved hard X-ray photoelectron spectroscopy analysis revealed that oxygen vacancies in IGZO:H were much fewer than those in IGZO, especially in the region near the film surface. Moreover, it was found that the density of near-conduction band minimum states in IGZO:H was lower than that in IGZO. Therefore, IGZO:H played a key role in improving the Schottky interface quality, namely, the increase of Schottky barrier height, decrease of oxygen vacancies, and reduction of near-conduction band minimum states. Finally, we fabricated a flexible IGZO:H SD on a poly(ethylene naphthalate) substrate, and it exhibited record electrical properties with a rectification ratio of 1.7 × 109, Schottky barrier height of 1.12 eV, and ideality factor of 1.10. To the best of our knowledge, both the IGZO:H SDs formed on glass and poly(ethylene naphthalate) substrates achieved the best performance among the IGZO SDs reported to date. The proposed method successfully demonstrated great potential for future flexible electronic applications.

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Due to the characteristics of high electron mobility, ambient stability, proper energy level, and low processing temperature, zinc oxide (ZnO) has become a very promising electron transport material for photovoltaics. However, perovskite solar cells fabricated with ZnO reveal low efficiency because perovskite crystals may decompose thermally on the surface of ZnO as a result of proton transfer reactions. In this study, we are the first to incorporate an inexpensive, non-toxic polyethylene glycol (PEG) into ZnO and explore the passivation effect on the electron transport layer of perovskite solar cells. Suspension stability, surface roughness, electrical conductivity, crystal size, and photovoltaic properties with respect to the PEG incorporation are analyzed. The experimental results revealed that PEG incorporation effectively passivated the surface defects of ZnO, increased the electrical conductivity, and suppressed the charge recombination. The photocurrent density could increase from 15.2 to 19.2 mA/cm2, an increase of 27%.

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The facile sequential deposition of functional organic thin films by solution processes is critical for the development of a variety of high-performance organic devices without restriction in terms of materials and processes. Herein, we propose a simple fabrication process that entails stacking multiple layers of functional polymers to fabricate organic field-effect transistors (OFETs). The process involves stamping organic semiconducting layers formed on the surface of water onto a commonly used polymeric dielectric layer. Our scheme makes it possible to independently optimize organic semiconductor films by controlling the solvent evaporation time during the process of film formation on the surface of water. This approach eliminates the need to be concerned about any interference with adjacent layers. Utilizing this process, the fabrication of high-performance bottom-gated OFETs is demonstrated on a glass and a flexible substrate. The OFETs consist of a vertically stacked diketopyrrolopyrrole-based polymer semiconducting layer on the poly(methyl methacrylate) film with a maximum hole mobility of 0.85 cm2/V s.

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An Nb-doped TiO2 (Nb-TiO2) film comprising a double structure stacked with a bottom compact layer and top mesoporous layers was synthesized by treating a Ti precursor-coated substrate using a one-step low-temperature steam-annealing (SA) method. The SA-based Nb-TiO2 films possess high crystallinity and conductivity, and that allows better control over the conduction band (CB) of TiO2 for the electron transport layer (ETL) of the perovskite solar cells by the Nb doping level. Optimization of power conversion efficiency (PCE) for the Nb-TiO2-based ETL was combined with the CB level tuning of the mixed-halide perovskite by changing the Br/I ratio. This band offset management enabled to establish the most suitable energy levels between the ETL and the perovskites. This method was applied to reduce the band gap of perovskites to enhance the photocurrent density while maintaining a high open-circuit voltage. As a result, the optimal combination of 5 mol % Nb-TiO2 ETL and 10 mol % Br in the mixed-halide perovskite exhibited high photovoltaic performance for low-temperature device fabrication, achieving a high-yield PCE of 21.3%.

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Perovskite solar cells (PSCs), which have surprisingly emerged in recent years, are now aiming at commercialization. Rapid, low-temperature, and continuous fabrication processes that can produce high-efficiency PSCs with a reduced fabrication cost and shortened energy payback time are important challenges on the way to commercialization. Herein, we report a reactive ion etching (RIE) method, which is an ultrafast room-temperature technique, to fabricate mesoporous TiO2 (mp-TiO2) as an electron transport layer for high-efficiency PSCs. Replacing the conventional high-temperature annealing process by RIE reduces the total processing time for fabricating 20 PSCs by 40%. Additionally, the RIE-processed mp-TiO2 exhibits enhanced electron extraction, whereupon the optimized RIE-mp-TiO2-based PSC exhibits a power conversion efficiency (PCE) of 19.60% without J-V hysteresis, when the devices were optimized with a TiCl4 surface treatment process. Finally, a flexible PSC employing RIE-mp-TiO2 is demonstrated with 17.29% PCE. Considering that the RIE process has been actively used in the semiconductor industry, including for the fabrication of silicon photovoltaic modules, the process developed in this work could be easily applied toward faster, simpler, and cheaper manufacturing of PSC modules.

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PbSe colloidal quantum dots (CQDs) are widely used in solar cells because of their tunable band gap, solution processability, and efficient multiple exciton generation effect. The most efficient PbSe CQD solar cells use high-temperature-processed ZnO as the electron transport layer (ETL), limiting their applications in flexible photovoltaics. Currently, low-temperature solution-processed SnO2 has been demonstrated as an efficient ETL for high-efficient PbS CQD and perovskite solar cells because of less parasitic light absorption and higher electron mobility. Herein, we introduce low-temperature solution-processed SnO2 as ETL for PbSe CQD solar cells, and fabricate the PbSe CQD absorber layer with a one-step spin-coating method. The champion device with the structure of FTO (SnO2:F)/SnO2/PbSe-PbI2/PbS-EDT (1,2-ethanedithiol)/Au achieves a high open-circuit voltage of 577.1 mV, a short-circuit current density of 24.87 mA cm-2, a fill factor of 67%, and an impressive power conversion efficiency of 9.67%. Our results pave the way for the development of low-temperature flexible PbSe CQD solar cells.

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During the manufacture of H1N1 microneedles, a stabilizer is usually added to maintain the antigenicity of the vaccine. However, finding a suitable stabilizer is difficult, and the addition of a stabilizer can limit the antigen dose and the addition of an adjuvant because of the limited volume of the microneedles. In this study, the authors evaluated whether H1N1 microneedles could be fabricated without a stabilizer by keeping the production environment at a low temperature. H1N1 microneedle patches without a stabilizer were prepared in a process that involved maintaining a low temperature of 10 °C. The protective immune response to this method of drug application was investigated by comparing it with traditional intramuscular (IM) immunization and with the use of H1N1 microneedles with a stabilizer. A process-sensitive antigen, H1N1, was stabilized without the use of a stabilizer in a process that maintained a low temperature of 10 °C. The preparation process consisted of coating and drying processes. In animal experiments, mice were immunized using an array of low-temperature H1N1 microneedles without a stabilizer (LT-MN), and they showed strong antibody responses. Compared to three other application methods of traditional IM immunization, low-temperature H1N1 microneedles with a stabilizer (LT-MN-T), and room-temperature H1N1 microneedles with a stabilizer (RT-MN-T), LT-MN produced comparable results in inducing protective immunity. A plaque reduction neutralization test found that LT-MN and LT-MN-T provided greater immunity compared with IM and RT-MN-T. A process in which the temperature is maintained at 10 °C can provide successful vaccination with H1N1 microneedles without the addition of a stabilizer. This process can be applied to various temperature-sensitive biologics.

Asunto(s)

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Achieving favorable band profile in low-temperature-grown Cu(In,Ga)Se2 thin films has been challenging due to the lack of thermal diffusion. Here, by employing a thin Ag precursor layer, we demonstrate a simple co-evaporation process that can effectively control the Ga depth profile in CIGS films at low temperature. By tuning the Ag precursor thickness (∼20 nm), typical V-shaped Ga gradient in the copper indium gallium diselenide (CIGS) film could be substantially mitigated along with increased grain sizes, which improved the overall solar cell performance. Structural and compositional analysis suggests that formation of liquid Ag-Se channels along the grain boundaries facilitates Ga diffusion and CIGS recrystallization at low temperatures. Formation of a fine columnar grain structure in the first evaporation stage was beneficial for subsequent Ga diffusion and grain coarsening. Compared to the modified co-evaporation process where the Ga evaporation profile has been directly tuned, the Ag precursor approach offers a convenient route for absorber engineering and is potentially more applicable for roll-to-roll fabrication system.

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Artificial synapses are the fundamental of building a neuron network for neuromorphic computing to overcome the bottleneck of the von Neumann system. Based on a low-temperature atomic layer deposition process, a flexible electrical synapse was proposed and showed bipolar resistive switching characteristics. With the formation and rupture of ions conductive filaments path, the conductance was modulated gradually. Under a series of pre-synaptic spikes, the device successfully emulated remarkable short-term plasticity, long-term plasticity, and forgetting behaviors. Therefore, memory and learning ability were integrated to the single flexible memristor, which are promising for the next-generation of artificial neuromorphic computing systems.

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Tin dioxide (SnO2) as an efficient electron transport layer (ETL) has been demonstrated for emerging high-performance organic-inorganic hybrid perovskite solar cells (PSCs). However, the low-temperature solution-processed SnO2 usually results in high trap-state density and current-voltage hysteresis. Here, we reported an effective strategy to solve this problem by incorporating graphene ink into the low-temperature processed SnO2 for planar structure PSCs. The electron extraction efficiency has been significantly improved with graphene-doped SnO2 ETL coupled with attenuated charge recombination at the ETL/perovskite interface. The power conversion efficiency (PCE) of PSCs based on the graphene-SnO2 ETL reached over 18% with negligible hysteresis. Incorporation of graphene into the ETL layer also enhanced the device stability retaining 90% of the initial PCE value after storing in ambient condition with a relative humidity of 40 ± 5% for 300 h. Our results provide an important insight into further efficiency boost in SnO2-based low-temperature processed PSCs.

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In the past few years, substantial progress has been made in perovskite light-emitting devices. Both pure green and infrared thin-film perovskite light-emitting devices with external quantum efficiency over 20% have been successfully achieved. However, pure-red and blue thin-film perovskite light-emitting diodes still suffer from inferior efficiency. Therefore, the development of efficient and stable thin-film perovskite light-emitting diodes with pure-red and blue emissions is urgently needed for possible applications as a new display technology and solid-state lighting. Here, we demonstrate an efficient light-emitting diode with pure-red emission based on polymer-assisted in situ growth of high-quality all-inorganic CsPbBr0.6I2.4 perovskite nanocrystal films with homogenous distribution of nanocrystals with size 20-30 nm. With this method, we can dramatically reduce the formation temperature of CsPbBr0.6I2.4 and stabilize its perovskite phase. Eventually, we successfully demonstrate a pure-red-emission perovskite light-emitting diode with a high external quantum efficiency of 6.55% and luminance of 338 cd/m2. Furthermore, the device obtains an ultralow turn-on voltage of 1.5 V and a half-lifetime of over 0.5 h at a high initial luminance of 300 cd/m2.