Ferroelectric Hafnia-Based M3D FeTFTs Annealed at Extremely Low Temperatures and TCAM Cells for Computing-in-Memory Applications.

In order to overcome the bottleneck between the central processor unit and memory as well as the issue of energy consumption, computing-in-memory (CIM) is becoming more popular as an alternative to the traditional von Neumann structure. However, as artificial intelligence advances, the networks require CIM devices to store billions of parameters in order to handle huge data traffic demands. Monolithic three-dimensional (M3D) stacked ferroelectric thin-film transistors (FeTFTs) are one of the promising techniques for realizing high-density CIM devices that can store billions of parameters. In particular, oxide channel-based FeTFTs are well suited for these applications due to low-temperature processes, nonvolatility, and 3D integration capability. Nevertheless, the M3D-integrated CIM devices including hafnia ferroelectric films need the high-temperature annealing process to crystallize the ferroelectric layer, making M3D integration difficult. When the FeTFTs are fabricated with an M3D structure, the high-temperature process causes thermal issues in the underlying devices. Here, we present the focused microwave annealed (FMA) oxide FeTFTs with M3D integration at a low temperature of 250 °C. We confirmed that the FeTFTs with metal-ferroelectric-metal-insulator-semiconductor structure exhibited a large memory window of 3.2 V, good endurance over 106 cycles, and a long retention time of 105 s. To understand the different electrical characteristics of FeTFTs in the top and bottom layers, we experimentally analyzed the density of the state of the oxide channel and ferroelectric properties of the ferroelectric gate insulator by using multifrequency capacitance-voltage measurement and nucleation-limited-switching model analysis, respectively. With our approach, we demonstrate for the first time a vertical stacked FeTFTs-based ternary-content-addressable memory (TCAM) cell for CIM application. We believe that the proposed M3D-stacked TCAM cells composed of FeTFTs can be used in high-density memory, energy-efficient memory, and CIM technology.

Power-Delay Area-Efficient Processing-In-Memory Based on Nanocrystalline Hafnia Ferroelectric Field-Effect Transistors.

Ferroelectric field-effect transistors (FeFETs) have attracted enormous attention for low-power and high-density nonvolatile memory devices in processing-in-memory (PIM). However, their small memory window (MW) and limited endurance severely degrade the area efficiency and reliability of PIM devices. Herein, we overcome such challenges using key approaches covering from the material to the device and array architecture. High ferroelectricity was successfully demonstrated considering the thermodynamics and kinetics, even in a relatively thick (≥30 nm) ferroelectric material that was unexplored so far. Moreover, we employed a metal-ferroelectric-metal-insulator-semiconductor architecture that enabled desirable voltage division between the ferroelectric and the metal-oxide-semiconductor FET, leading to a large MW (∼11 V), fast operation speed (<20 ns), and high endurance (∼1011 cycles) characteristics. Subsequently, reliable and energy-efficient multiply-and-accumulation (MAC) operations were verified using a fabricated FeFET-PIM array. Furthermore, a system-level simulation demonstrated the high energy efficiency of the FeFET-PIM array, which was attributed to charge-domain computing. Finally, the proposed signed weight MAC computation achieved high accuracy on the CIFAR-10 dataset using the VGG-8 network.

A review on morphotropic phase boundary in fluorite-structure hafnia towards DRAM technology.

In the present hyper-scaling era, memory technology is advancing owing to the demand for high-performance computing and storage devices. As a result, continuous work on conventional semiconductor-process-compatible ferroelectric memory devices such as ferroelectric field-effect transistors, ferroelectric random-access memory, and dynamic random-access memory (DRAM) cell capacitors is ongoing. To operate high-performance computing devices, high-density, high-speed, and reliable memory devices such as DRAMs are required. Consequently, considerable attention has been devoted to the enhanced high dielectric constant and reduced equivalent oxide thickness (EOT) of DRAM cell capacitors. The advancement of ferroelectric hafnia has enabled the development of various devices, such as ferroelectric memories, piezoelectric sensors, and energy harvesters. Therefore, in this review, we focus the morphotropic phase boundary (MPB) between ferroelectric orthorhombic and tetragonal phases, where we can achieve a high dielectric constant and thereby reduce the EOT. We also present the role of the MPB in perovskite and fluorite structures as well as the history of the MPB phase. We also address the different approaches for achieving the MPB phase in a hafnia material system. Subsequently, we review the critical issues in DRAM technology using hafnia materials. Finally, we present various applications of the hafnia material system near the MPB, such as memory, sensors, and energy harvesters.

Novel Approach to High κ (∼59) and Low EOT (∼3.8 Å) near the Morphotrophic Phase Boundary with AFE/FE (ZrO2/HZO) Bilayer Heterostructures and High-Pressure Annealing.

We present herewith a novel approach of equally thick AFE/FE (ZrO2/HZO) bilayer stack heterostructure films for achieving an equivalent oxide thickness (EOT) of 4.1 Å with a dielectric constant (κ) of 56 in complementary metal-oxide semiconductor (CMOS) compatible metal-ferroelectric-metal (MFM) capacitors using a high-pressure annealing (HPA) technique. The low EOT and high κ values were achieved by careful optimization of AFE/FE film thicknesses and HPA conditions near the morphotropic phase boundary (MPB) after field cycling effects. Stable leakage current density (J < 10-7 A/cm2 at ±0.8 V) was found at 3/3 nm bilayer stack films (κ = 56 and EOT = 4.1 Å) measured at room temperature. In comparison with previous work, our remarkable achievement stems from the interfacial coupling between FE and AFE films as well as a high-quality crystalline structure formed by HPA. Kinetically stabilized hafnia films result in a small grain size in bilayer films, leading to reducing the leakage current density. Further, a higher κ value of 59 and lower EOT of 3.4 Å were found at 333 K. However, stable leakage current density was found at 273 K with a high κ value of 53 and EOT of 3.85 Å with J < 10-7 A/cm2. This is the lowest recorded EOT employing hafnia and TiN electrodes that are compatible with CMOS, and it has important implications for future dynamic random access memory (DRAM) technology.

Flexible Ferroelectric Hafnia-Based Synaptic Transistor by Focused-Microwave Annealing.

Hafnia-based ferroelectric memory devices with excellent ferroelectricity, low power consumption, and fast operation speed have attracted considerable interest with the ever-growing desire for nonvolatile memory in flexible electronics. However, hafnia films are required to perform a high temperature (>500 °C) annealing process for crystallization into the ferroelectric orthorhombic phase. It can hinder the integration of hafnia ferroelectric films on flexible substrates including plastic and polymer, which are not endurable at high temperatures above 300 °C. Here, we propose the extremely low-temperature (∼250 °C) process for crystallization of Hf0.5Zr0.5O2 (HZO) thin films by applying a focused-microwave induced annealing method. HZO thin films on a flexible mica substrate exhibits robust remnant polarization (2Pr ∼ 50 µC/cm2), which is negligibly changed under bending tests. In addition, the electrical characteristics of a HZO capacitor on the mica substrate were evaluated, and ferroelectric thin film transistors (Fe-TFTs), using a HZO gate insulator, were fabricated on mica substrates for flexible synapse applications. Symmetric potentiation and depression characteristics are successfully demonstrated in the Fe-TFT memory devices, and the synaptic devices result in high recognition accuracy of 91.44%. The low-temperature annealing method used in this work are promising for forming hafnia-based Fe-TFT memory devices as a building block on a flexible platform.

Selector-less Ferroelectric Tunnel Junctions by Stress Engineering and an Imprinting Effect for High-Density Cross-Point Synapse Arrays.

In the quest for highly scalable and three-dimensional (3D) stackable memory components, ferroelectric tunnel junction (FTJ) crossbar architectures are promising technologies for nonvolatile logic and neuromorphic computing. Most FTJs, however, require additional nonlinear devices to suppress sneak-path current, limiting large-scale arrays in practical applications. Moreover, the giant tunneling electroresistance (TER) remains challenging due to their inherent weak polarization. Here, we present that the employment of a diffusion barrier layer as well as a bottom metal electrode having a significantly low thermal expansion coefficient has been identified as an important way to enhance the strain, stabilize the ferroelectricity, and manage the leakage current in ultrathin hafnia film, achieving a high TER of 100, negligible resistance changes even up to 108 cycles, and a high switching speed of a few tens of nanoseconds. Also, we demonstrate that the usage of an imprinting effect in a ferroelectric capacitor induced by an ionized oxygen vacancy near the electrode results in highly asymmetric current-voltage characteristics with a rectifying ratio of 1000. Notably, the proposed FTJ exhibits a high density array size (>4k) with a securing read margin of 10%. These findings provide a guideline for the design of high-performance and selector-free FTJ devices for large-scale crossbar arrays in neuromorphic applications.

Transparent and Flexible Mayan-Pyramid-based Pressure Sensor using Facile-Transferred Indium tin Oxide for Bimodal Sensor Applications.

Transparent and conducting flexible electrodes have been successfully developed over the last few decades due to their potential applications in optoelectronics. However, recent developments in smart electronics, such as a direct human-machine interface, health-monitoring devices, motion-tracking sensors, and artificially electronic skin also require materials with multifunctional properties such as transparency, flexibility and good portability. In such devices, there remains room to develop transparent and flexible devices such as pressure sensors or temperature sensors. Herein, we demonstrate a fully transparent and flexible bimodal sensor using indium tin oxide (ITO), which is embedded in a plastic substrate. For the proposed pressure sensor, the embedded ITO is detached from its Mayan-pyramid-structured silicon mold by an environmentally friendly method which utilizes water-soluble sacrificial layers. The Mayan-pyramid-based pressure sensor is capable of six different pressure sensations with excellent sensitivity in the range of 100 Pa-10 kPa, high endurance of 105 cycles, and good pulse detection and tactile sensing data processing capabilities through machine learning (ML) algorithms for different surface textures. A 5 × 5-pixel pressure-temperature-based bimodal sensor array with a zigzag-shaped ITO temperature sensor on top of it is also demonstrated without a noticeable interface effect. This work demonstrates the potential to develop transparent bimodal sensors that can be employed for electronic skin (E-skin) applications.

Scalable and facile synthesis of stretchable thermoelectric fabric for wearable self-powered temperature sensors.

Wearable sensor systems with ultra-thinness, light weight, high flexibility, and stretchability that are conformally in contact with the skin have advanced tremendously in many respects, but they still face challenges in terms of scalability, processibility, and manufacturability. Here, we report a highly stretchable and wearable textile-based self-powered temperature sensor fabricated using commercial thermoelectric inks. Through various combinations of poly(3,4-ethylene dioxythiophene)-poly(styrene sulfonate) (PEDOT:PSS), silver nanoparticles (AgNPs), and graphene inks, we obtained linear temperature-sensing capability. The optimized sensor generates a thermoelectric voltage output of 1.1 mV for a temperature difference of 100 K through a combination of PEDOT:PSS and AgNPs inks and it shows high durability up to 800 cycles of 20% strain. In addition, the knitted textile substrate exhibits temperature-sensing properties that are dependent upon the stretching directions. We believe that stretchable thermoelectric fabric has broader potential for application in human-machine interfaces, health-monitoring technologies, and humanoid robotics.

Vertically stacked nanocellulose tactile sensor.

Paper-based electronic devices are attracting considerable attention, because the paper platform has unique attributes such as flexibility and eco-friendliness. Here we report on what is claimed to be the firstly fully integrated vertically-stacked nanocellulose-based tactile sensor, which is capable of simultaneously sensing temperature and pressure. The pressure and temperature sensors are operated using different principles and are stacked vertically, thereby minimizing the interference effect. For the pressure sensor, which utilizes the piezoresistance principle under pressure, the conducting electrode was inkjet printed on the TEMPO-oxidized-nanocellulose patterned with micro-sized pyramids, and the counter electrode was placed on the nanocellulose film. The pressure sensor has a high sensitivity over a wide range (500 Pa-3 kPa) and a high durability of 104 loading/unloading cycles. The temperature sensor combines various materials such as poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS), silver nanoparticles (AgNPs) and carbon nanotubes (CNTs) to form a thermocouple on the upper nanocellulose layer. The thermoelectric-based temperature sensors generate a thermoelectric voltage output of 1.7 mV for a temperature difference of 125 K. Our 5 × 5 tactile sensor arrays show a fast response, negligible interference, and durable sensing performance.

Paper-Based Bimodal Sensor for Electronic Skin Applications.

We present the development of a flexible bimodal sensor using a paper platform and inkjet printing method, which are suited for low-cost fabrication processes and realization of flexible devices. In this study, we employed a vertically stacked bimodal device architecture in which a temperature sensor is stacked on top of a pressure sensor and operated on different principles, allowing the minimization of interference effects. For the temperature sensor placed in the top layer, we used the thermoelectric effect and formed a closed-loop thermocouple composed of two different printable inks (conductive PEDOT:PSS and silver nanoparticles on a flexible paper platform) and obtained temperature-sensing capability over a wide range (150 °C). For the pressure sensor positioned in the bottom layer, we used microdimensional pyramid-structured poly(dimethylsiloxane) coated with multiwall carbon nanotube conducting ink. Our pressure sensor exhibits a high-pressure sensitivity over a wide range (100 Pa to 5 kPa) and high-endurance characteristics of 105. Our 5 × 5 bimodal sensor array demonstrates negligible interference, high-speed responsivity, and robust sensing characteristics. We believe that the material, process, two-terminal device, and integration scheme developed in this study have a great value that can be widely applied to electronic skin.

Cell Electrical Impedance as a Novel Approach for Studies on Senescence Not Based on Biomarkers.

Senescence of cardiac myocytes is frequently associated with heart diseases. To analyze senescence in cardiac myocytes, a number of biomarkers have been isolated. However, due to the complex nature of senescence, multiple markers are required for a single assay to accurately depict complex physiological changes associated with senescence. In single cells, changes in both cytoplasm and cell membrane during senescence can affect the changes in electrical impedance. Based on this phenomenon, we developed MEDoS, a novel microelectrochemical impedance spectroscopy for diagnosis of senescence, which allows us to precisely measure quantitative changes in electrical properties of aging cells. Using cardiac myocytes isolated from 3-, 6-, and 18-month-old isogenic zebrafish, we examined the efficacy of MEDoS and showed that MEDoS can identify discernible changes in electrical impedance. Taken together, our data demonstrated that electrical impedance in cells at different ages is distinct with quantitative values; these results were comparable with previously reported ones. Therefore, we propose that MEDoS be used as a new biomarker-independent methodology to obtain quantitative data on the biological senescence status of individual cells.