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Microembossing: A Convenient Process for Fabricating Microchannels on Nanocellulose Paper-Based Microfluidics

Nanopaper, derived from nanofibrillated cellulose, has generated considerable interest as a promising material for microfluidic applications. Its appeal ...

University of Liverpool

Ellipsometry was used to measure the amplitude ratio and phase difference of light undergoing a phase shift as it interacts with a thin film of organic-inorganic hybrid perovskite CH3NH3PbI3 (MAPI) deposited onto a (100) silicon wafer. The refractive index and extinction coefficient was extracted from a multi-oscillator model fit to the ellipsometry data, as a function of wavelength, from 300 to 1500 nm.

Dispersion relation data for methylammonium lead triiodide perovskite deposited on a (100) silicon wafer using a two-step vapour-phase reaction process.

In this research, the hafnium titanate oxide thin films, TiHfO₂, with titanium contents of  = 0, 0.25, 0.9, and 1 were deposited on germanium substrates by atomic layer deposition (ALD) at 300 °C. The approximate deposition rates of 0.2 Å and 0.17 Å per cycle were obtained for titanium oxide and hafnium oxide, respectively. X-ray Photoelectron Spectroscopy (XPS) indicates the formation of GeO and germanate at the interface. X-ray diffraction (XRD) indicates that all the thin films remain amorphous for this deposition condition. The surface roughness was analyzed using an atomic force microscope (AFM) for each sample. The electrical characterization shows very low hysteresis between ramp up and ramp down of the Capacitance-Voltage (CV) and the curves are indicative of low trap densities. A relatively large leakage current is observed and the lowest leakage current among the four samples is about 1 mA/cm² at a bias of 0.5 V for a TiHfO₂ sample. The large leakage current is partially attributed to the deterioration of the interface between Ge and TiHfO₂ caused by the oxidation source from HfO₂. Consideration of the energy band diagrams for the different materials systems also provides a possible explanation for the observed leakage current behavior.

Electrical Properties and Interfacial Studies of HfTiO₂ High Permittivity Gate Insulators Deposited on Germanium Substrates.

Resistive random access memory (RRAM) devices with Ni/AlO/Pt-structure were manufactured by deposition of a solution-based aluminum oxide (AlO) dielectric layer which was subsequently annealed at temperatures from 200 °C to 300 °C, in increments of 25 °C. The devices displayed typical bipolar resistive switching characteristics. Investigations were carried out on the effect of different annealing temperatures for associated RRAM devices to show that performance was correlated with changes of hydroxyl group concentration in the AlO thin films. The annealing temperature of 250 °C was found to be optimal for the dielectric layer, exhibiting superior performance of the RRAM devices with the lowest operation voltage (<1.5 V), the highest ON/OFF ratio (>10), the narrowest resistance distribution, the longest retention time (>10 s) and the most endurance cycles (>150).

Effect of Annealing Temperature for Ni/AlO/Pt RRAM Devices Fabricated with Solution-Based Dielectric.

Resistive random access memory (RRAM), which is considered as one of the most promising next-generation non-volatile memory (NVM) devices and a representative of memristor technologies, demonstrated great potential in acting as an artificial synapse in the industry of neuromorphic systems and artificial intelligence (AI), due its advantages such as fast operation speed, low power consumption, and high device density. Graphene and related materials (GRMs), especially graphene oxide (GO), acting as active materials for RRAM devices, are considered as a promising alternative to other materials including metal oxides and perovskite materials. Herein, an overview of GRM-based RRAM devices is provided, with discussion about the properties of GRMs, main operation mechanisms for resistive switching (RS) behavior, figure of merit (FoM) summary, and prospect extension of GRM-based RRAM devices. With excellent physical and chemical advantages like intrinsic Young's modulus (1.0 TPa), good tensile strength (130 GPa), excellent carrier mobility (2.0 × 10 cm∙V∙s), and high thermal (5000 Wm∙K) and superior electrical conductivity (1.0 × 10 S∙m), GRMs can act as electrodes and resistive switching media in RRAM devices. In addition, the GRM-based interface between electrode and dielectric can have an effect on atomic diffusion limitation in dielectric and surface effect suppression. Immense amounts of concrete research indicate that GRMs might play a significant role in promoting the large-scale commercialization possibility of RRAM devices.

Memristive Non-Volatile Memory Based on Graphene Materials.

Resistive random access memory (RRAM) devices are receiving increasing extensive attention due to their enhanced properties such as fast operation speed, simple device structure, low power consumption, good scalability potential and so on, and are currently considered to be one of the next-generation alternatives to traditional memory. In this review, an overview of RRAM devices is demonstrated in terms of thin film materials investigation on electrode and function layer, switching mechanisms and artificial intelligence applications. Compared with the well-developed application of inorganic thin film materials (oxides, solid electrolyte and two-dimensional (2D) materials) in RRAM devices, organic thin film materials (biological and polymer materials) application is considered to be the candidate with significant potential. The performance of RRAM devices is closely related to the investigation of switching mechanisms in this review, including thermal-chemical mechanism (TCM), valance change mechanism (VCM) and electrochemical metallization (ECM). Finally, the bionic synaptic application of RRAM devices is under intensive consideration, its main characteristics such as potentiation/depression response, short-/long-term plasticity (STP/LTP), transition from short-term memory to long-term memory (STM to LTM) and spike-time-dependent plasticity (STDP) reveal the great potential of RRAM devices in the field of neuromorphic application.

Advances of RRAM Devices: Resistive Switching Mechanisms, Materials and Bionic Synaptic Application.

The ecofriendly combustion synthesis (ECS) and self-combustion synthesis (ESCS) have been successfully utilized to deposit high- aluminum oxide (AlO) dielectrics at low temperatures and applied for aqueous InO thin-film transistors (TFTs) accordingly. The ECS and ESCS processes facilitate the formation of high-quality dielectrics at lower temperatures compared to conventional methods based on an ethanol precursor, as confirmed by thermal analysis and chemical composition characterization. The aqueous InO TFTs based on ECS and ESCS-AlO show enhanced electrical characteristics and counterclockwise transfer-curve hysteresis. The memory-like counterclockwise behavior in the transfer curve modulated by the gate bias voltage is comparable to the signal modulation by the neurotransmitters. ECS and ESCS transistors are employed to perform synaptic emulation; various short-term and long-term memory functions are emulated with low operating voltages and high excitatory postsynaptic current levels. High stability and reproducibility are achieved within 240 pulses of long-term synaptic potentiation and depression. The synaptic emulation functions achieved in this work match the demand for artificial neural networks (ANN), and a multilayer perceptron (MLP) is developed using an ECS-AlO synaptic transistor for image recognition. A superior recognition rate of over 90% is achieved based on ECS-AlO synaptic transistors, which facilitates the implementation of the metal-oxide synaptic transistor for future neuromorphic computing via an ecofriendly route.

Ecofriendly Solution-Combustion-Processed Thin-Film Transistors for Synaptic Emulation and Neuromorphic Computing.

The quest to harvest untapped renewable infrared energy sources has led to significant research effort in design, fabrication and optimization of a self-biased rectenna that can operate without external bias voltage. At the heart of its design is the engineering of a high-frequency rectifier that can convert terahertz and infrared alternating current (AC) signals to usable direct current (DC). The Metal Insulator Metal (MIM) diode has been considered as one of the ideal candidates for the rectenna system. Its unparalleled ability to have a high response time is due to the fast, femtosecond tunneling process that governs current transport. This paper presents an overview of single, double and triple insulator MIM diodes that have been fabricated so far, in particular focusing on reviewing key figures of merit, such as zero-bias responsivity (), zero-bias dynamic resistance () and asymmetry. The two major oxide contenders for MIM diodes have been NiO and AlO, in combination with HfO, TaO, NbO, ZnO and TiO. The latter oxide has also been used in combination with CoO and TiO. The most advanced rectennas based on MIM diodes have shown that optimal ( and ) can be achieved by carefully tailoring fabrication processes to control oxide stoichiometry and thicknesses to sub-nanometer accuracy.

Oxides for Rectenna Technology.

Radiation hardness is important for electronics operating in harsh radiation environments such as outer space and nuclear energy industries. In this work, radiation-hardened solution-processed ZrLaO thin films are demonstrated. The radiation effects on solution-processed ZrLaO thin films and InO/ZrLaO thin-film transistors (TFTs) were systemically investigated. The ZrLaO thin films demonstrated excellent radiation hardness with negligible roughness, composition, electrical property, and bias-stress stability degradation after radiation exposure. The metal-oxide-semiconductor capacitors (MOSCAPs) based on ZrLaO gate dielectrics exhibited an ultralow flat band-voltage () sensitivity of 0.11 mV/krad and 0.19 mV/krad under low dose and high dose gamma irradiation conditions, respectively. The low dose condition had a 103 krad (SiO) total dose and a 0.12 rad/s low dose rate, whereas the high dose condition had a 580 krad total dose and a 278 rad/s high dose rate. Furthermore, InO/ZrLaO thin-film transistors (TFTs) exhibited a large / of 2 × 10, a small subthreshold swing (SS) of 0.11 V/dec, a small interface trap density () of 1 × 10 cm, and a 0.16 V threshold shift (Δ) under 3600 s positive bias-stress (PBS). InO/ZrLaO TFT-based resistor-loaded inverters demonstrated complete swing behavior, a static output gain of 13.3 under 4 V , and an ∼9% radiation-induced degradation. Through separate investigation of the radiation-induced degradation on the semiconductor layer and dielectric layer of TFTs, it was found that radiation exposure mainly generated oxygen vacancies (V) and increased electron concentration among gate oxide. Nevertheless, the radiation-induced TFT instability was mainly related to the semiconductor layer degradation, which could be possibly suppressed by back-channel passivation. The demonstrated results indicate that solution-processed ZrLaO is a high-potential candidate for large-area electronics and circuits applied in harsh radiation environments. In addition, the detailed investigation of radiation-induced degradation on solution-processed high- dielectrics in this work provided clear inspiration for developing novel flexible rad-hard dielectrics.

High-Performance and Radiation-Hardened Solution-Processed ZrLaO Gate Dielectrics for Large-Area Applications.

Nanofibrillated cellulose paper (nanopaper) has gained growing interest as one promising substrate material for paper-based microfluidics, thanks to its ultrasmooth surface, high optical transparency, uniform nanofiber matrix with nanoscale porosity, and tunable chemical properties. Recently, research on nanopaper-based microfluidics has quickly advanced; however, the current technique of patterning microchannels on nanopaper (i.e., 3D printing, spray coating, or manual cutting and sticking), that is fundamental for application development, still has some limitations, such as ease-of-contamination, and more importantly, only enabling millimeter-scale channels. This paper reports a facile process that leverages the simple operations of microembossing with the convenient plastic micro-molds, for the first time, patterning nanopaper microchannels downing to 200 μm, which is 4 times better than the existing methods and is time-saving (<45 mins). We also optimized the patterning parameters and provided one quick look-up table as the guideline for application developments. As proof-of-concept, we first demonstrated two fundamental microfluidic devices on nanopaper, the laminar-mixer and droplet generator, and two functional nanopaper-based analytical devices (NanoPADs) for glucose and Rhodamine B (RhB) sensing based on optical colorimetry and surface-enhanced Raman spectroscopy, respectively. The two NanoPADs showed outstanding performance with low limits of detection (2 mM for glucose and 19fM for RhB), which are 1.25× and 500× fold improvement compared to the previously reported values. This can be attributed to our newly developed highly accurate microchannel patterning process that enables high integration and fine-tunability of the NanoPADs along with the superior optical properties of nanopaper.

Article	Year
Dispersion relation data for methylammonium lead triiodide perovskite deposited on a (100) silicon wafer using a two-step vapour-phase reaction process. Data in brief\| PubMed ID: 26702423	2015
Electrical Properties and Interfacial Studies of HfTiO₂ High Permittivity Gate Insulators Deposited on Germanium Substrates. Materials (Basel, Switzerland)\| PubMed ID: 28793705	2015
Effect of Annealing Temperature for Ni/AlO/Pt RRAM Devices Fabricated with Solution-Based Dielectric. Micromachines\| PubMed ID: 31269730	2019
Memristive Non-Volatile Memory Based on Graphene Materials. Micromachines\| PubMed ID: 32218324	2020
Advances of RRAM Devices: Resistive Switching Mechanisms, Materials and Bionic Synaptic Application. Nanomaterials (Basel, Switzerland)\| PubMed ID: 32717952	2020
Ecofriendly Solution-Combustion-Processed Thin-Film Transistors for Synaptic Emulation and Neuromorphic Computing. ACS applied materials & interfaces\| PubMed ID: 33848133	2021
Oxides for Rectenna Technology. Materials (Basel, Switzerland)\| PubMed ID: 34576441	2021
High-Performance and Radiation-Hardened Solution-Processed ZrLaO Gate Dielectrics for Large-Area Applications. ACS applied materials & interfaces\| PubMed ID: 34636544	2021
Facile Microembossing Process for Microchannel Fabrication for Nanocellulose-Paper-Based Microfluidics. ACS applied materials & interfaces\| PubMed ID: 36693010	2023

Ivona Mitrovic

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