United States

Abstract Body: Resistive switching memory devices are being widely studied due to their excellent characteristics such as high scalability, non-volatility, and fast operation speed. Organo-metal halide perovskite (OHP), which is solution-processable and has outstanding optical and electrical properties, is also applied to a resistive memory device. OHP resistive memory has the advantage of being able to operate with a low voltage and large ON/OFF ratio [1]. On the other hand, random distribution in operation voltage remains a challenge in memory application. This stochastic operation characteristic is due to the random formation of conducting filaments that cause resistance changes in the material. Therefore, studies on the structure of the conducting filament are important. However, observing a nano-scale structure is difficult. Moreover, there is insufficient research on how the conducting filaments are formed in OHP materials. In this presentation, the geometric shape of the conducting filaments formed in the perovskite was explored through a current noise analysis. By observing the electrical properties and current noise under different temperature conditions, we investigated how the temperature condition affects the formation of the conductive filaments [2]. Through this, more advanced understanding of the operating mechanism of the perovskite resistive memory device will be possible. References [1] K. Kang, H. Ahn et al., Adv. Mater. 31, 1804841 (2019). [2] H. Ahn et al., manuscript in preparation.

EMC 2021

Current Noise Analysis on Organo-Metal Halide Perovskite Resistive Switching Memory

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Abstract Body: Alloys made of III-nitrides such as GaN, AlN, InN have been and continue to be of large technological and economic importance. They have found use in devices such as light-emitting diodes and High Electron Mobility Transistors. However, lattice mismatches limit the performance of III-nitride-based devices. One proposed solution that has received interest in recent years is the incorporation of ScN to enhance optical and electronic properties. In particular, scandium aluminum nitride (ScxAl1-xN) has been demonstrated to exhibit spontaneous polarization, high piezoelectricity, a wide bandgap, and an excellent lattice match to GaN. These properties have been demonstrated to be dependent on the Sc content and growth parameters such as temperature, pressure, and sputtering mode. ScxAl1-xN-based devices are expected to find use in applications such as filters and resonators, microelectromechanical systems and transistors, among others. This work reports the characterization of ScxAl1-xN films deposited on oxidized silicon substrates by a pulsed DC magnetron sputtering technique. The Sc and Al sources used were 99.999% pure Sc and 99.9995% pure Al targets. Sample composition and crystalline orientation were investigated using X-ray photoelectron spectroscopy and X-ray diffraction. Investigation on surface roughness was conducted using atomic force microscopy. Our results contribute to the understanding and development of ScxAl1-xN synthesis and characterization for the next generation of electronic devices and sensors.

Composition and Electrical Characterization of ScxAl1-xN Grown on Si Substrate by DC Sputtering

Abstract Body: The rapid increase in data quantity and processing necessitate novel approaches to computing. Digital computing based on von Neumann architectures may not be optimal for data-intensive operations like machine learning due to the high energy costs of moving data between processor and memory. Neuromorphic computing that combines logic and memory functionality into a single analogue nonvolatile memory element is a promising energy-efficient solution that decreases the energy consumption by orders of magnitude. Filament-based phase-change memory and resistive random access memory are the most well-investigated approaches to neuromorphic computing, but these memories are stochastic due to the unreliability of the nanosized filaments used to store information. In this work, we develop the “bulk” resistive random access memory that stores information using the oxygen vacancy concentration in the 3D bulk. This cell contains a solid electrolyte sandwiched between two mixed ionic and electronic conductors (MIECs). The ion-conducting solid electrolyte blocks electrons and prevents the positive feedback that results in filament formation. Instead, the oxygen vacancy ions are uniformly distributed in the absence of filaments and thermal gradients. To switch the cell, electrochemical voltage pulses (+/-1.5V, 2 μs) shuttle vacancies between the MIECs; the concentration of the vacancies in one MIEC stores the analogue resistive state. This enables exceptionally reliable, linear, and deterministic switching among hundreds of analogue information states, while utilizing CMOS-compatible materials with long endurance and information retention. Atomic force microscopy and physical modeling confirms the absence of filaments. Three types of solid electrolytes are utilized: a thick model single-crystal yttrium-stabilized zirconia (YSZ), a thin-film YSZ grown by sputtering, and ultra-thin-film electrolytes of alumina, hafnia, and zirconia grown by atomic layer deposition. The oxygen vacancy ionic conductivities of these materials play a crucial role in the switching and retention times. The broad classes of oxygen conductors provide significant opportunities for future materials research towards next-generation analogue nonvolatile memory. Reference: “Filament-free bulk resistive memory enables deterministic analogue switching,” Adv Mater, 32, 2003984 (2020)

Deterministic Analogue Resistive Memory for Neuromorphic Computing Based on Transition Metal Oxides

Abstract Body: Recently, research on wearable intelligent electronics that detects, remembers, and learns external stimuli in real-time is receiving great interest. And a tactile synaptic device studies have emerged because they have the potential for human-interactive neuromorphic applications capable of large-scale parallel processing. However, the artificial tactile synaptic devices reported so far have complex physical connections between the sensor unit and the memory unit, which are inevitably not suitable for the wearable and patchable device due to the complex and costly manufacturing steps. Here, we demonstrate an artificial organic tactile synaptic device based on the integrated single device that enables the sensing, storing, and learning of a variety of tactile information. The synaptic device is able to be programmed with various tactile input pressures, by using a ferroelectric field-effect transistor structure with a pressure-sensitive ball-shaped top gate electrode. The synaptic device reliably and stably operates with high tactile reception sensitivity of 88 KPa-1 under bending conditions. And it was confirmed that synaptic plasticity was stably implemented for 10,000 inputs by various electrical/tactile stimuli, which allows for precise and robust tactile perception learning. Furthermore, we demonstrated that an integrated 4 x 4 tactile synaptic array allows for 2-dimensional tactile learning and proof-of-concept recognition simulations for diverse handwriting patterns with an outstanding error tolerance. As a result, our study proposes the novel platform for a single, integrated tactile neuromorphic system, which can simultaneously sense and learn a variety of external information.

Development of a Single Device-Based Organic Tactile Synapse for Artificial Learning Skin Applications

Abstract Body: We report the observation of ferroelectricity in hafnium-zirconium-oxide thin films in the as-deposited state, namely after deposition at a low temperature of 300 °C without post-metallization annealing. The Hf0.5Zr0.5O2 (HZO) thin film was interposed between two TiO2 interlayers, and all films were produced by plasma enhanced atomic layer deposition and integrated into a TiN-based metal-insulator-metal capacitor. The ferroelectric nature of the as-deposited HZO film was evaluated by a polarization-voltage hysteresis loop and a 2Pr value of ~7.4 μC/cm2 was achieved. Grazing incidence x-ray diffraction measurements and atomic-resolution scanning transmission electron microscopy characterization revealed the co-existence of fully crystallized polar orthorhombic and monoclinic phases of the dielectric in the as-deposited sample. We concluded that the nucleation and growth of the crystalline polar non-centrosymmetric orthorhombic phases in the 10 nm HZO thin film was prompted by the available energy from the plasma and the tensile lattice mismatch strain provided by the TiO2 interlayer.

Ferroelectricity of As-Deposited HZO Fabricated by Plasma-Enhanced Atomic Layer Deposition at 300°C by Inserting TiO2 Interlayers

Abstract Body: Spin Hall materials provide an energy efficient way to flip the orientation of a neighbouring magnetic layer and this ability could form the basis of future low power, high endurance MRAM devices. A wide array of computational techniques has been developed to investigate and optimize the different intrinsic and extrinsic aspects of the spin Hall effect (SHE) in materials. In this study, we use the screened Korringa-Kohn-Rostocker (KKR) methods[1] along with the linearized Boltzmann Transport equation, Quantum Espresso[2] and PAOFLOW[3] to reveal how dilute N or O impurities affect both the intrinsic and extrinsic SHE in bcc and β phase tungsten[4]. Our results, when examined in combination, suggest that the formation of grain boundaries with the doped system plays an important role in amplifying the SHE in β tungsten. Beyond this particular system, further techniques such as the coherent potential approximation enables us to treat not only dilute but concentrated alloys as well. With this expanded tool set, an even wider array of other spintronic materials, such as Pt based alloys will be explored. [1] L. Peti et al, Philos. Mag. B 78, 449 (1998) [2] P. Gianozzi et al, J. Phys.: Condens. Matt. 21, 395502 (2009) [3] M. B. Nardelli et al, Comp. Mat. Sci. 143, 462-472 (2018) [4] O. L. W. McHugh, M. Gradhand, W. F. Goh and D. A. Stewart, Phys. Rev. Mat. 4, 094404 (2020)

Tackling the Total Spin Hall Conductivity—A Multi-Code Approach for Doped and Alloyed Materials

Abstract Body: Molecular Spintronics devices (MSD), which possess tunable spin states, are crucial for the advancement of futuristic quantum computing technology [1]. To overcome the dominant issue of reliable mass producibility for existing MSD technology, we have designed a magnetic tunnel junction based molecular spintronics device (MTJMSD). MTJMSD is fabricated by bridging paramagnetic molecules across the edges of the ferromagnetic electrodes to create spin channels. MTJMSD enables the utilization of ferromagnetic electrodes with a wide range of magnetic anisotropies. There is a knowledge gap about the role of magnetic anisotropy on the magnetic swicthing mechanism and equilibrium magnetic prperties of the MTJMSDs. Understanding the role of anisotropy is crucial to apply this technology in futuristic spin valve type memory device applications. In this study we investigated the effect of anisotropy on the nature of the hysteresis curves generated computationally using Monte Carlo Simulations (MCS). We applied the in-plane magnetic anisotropy () along the ferromagnetic electrode of a magnetic tunnel junction. The magnitude of A varied numerically from 0 to1. A=1 represented strong anisotropy of the order of interatomic Heisenberg exchange on the ferromagnetic electrodes. We also varied the thermal energy of the device from = 0.05 to 1.1. Here, = 0.1 corresponds to the operating temperature ranges from 500C to 900C with the assumption that the Curie temperature of the device lies between 5000C to 9000C. The effect of the anisotropy transformed the regular magnetic hysteresis of MTJMSD into a “wasp-waisted” -like hysteresis curve[2]. The “wasp-waisted” -like hysteresis curve is hypothesized due to the presence of multiple magnetic phases present on the ferromagnetic electrodes caused by strong magnetic anisotropy. Here, the materials possess hard and soft magnetic phases due to the higher and lower values of coercive fields. The “wasp-waisted” -like hysteresis curve was observed relatively at lower magnitudes of anisotropy at low thermal energy. The effect was observed up to = 0.8 with the high magnitude magnetic anisotropy ( 0.9). As a result, the effect of anisotropy keeps high magnetization of the device close to Curie temperature even when all the coupling effects get nullified due to thermal agitation. This research is supported by National Science Foundation-CREST Award (Contract # HRD- 1914751), Department of Energy/ National Nuclear Security Agency (DE-FOA-0003945). References [1] A. R. Rocha, V. M. García-suárez, S. W. Bailey, C. J. Lambert, J. Ferrer, and S. Sanvito, "Towards molecular spintronics," Nature Materials, vol. 4, no. 4, pp. 335-339, 2005/04/01 2005, doi: 10.1038/nmat1349. [2] T. M. de Lima Alves et al., "Wasp-waisted behavior in magnetic hysteresis curves of CoFe 2 O 4 nanopowder at a low temperature: Experimental evidence and theoretical approach," RSC advances, vol. 7, no. 36, pp. 22187-22196, 2017.

Impact of Anisotropy on the Magnetic Hysteresis of Magnetic Tunnel Junction Based Molecular Spintronics Device (MTJMSD) Properties

Abstract Body: A two-dimensional, solid-state, non-volatile memory has been demonstrated using electric double layer (EDL) gating of two-dimensional (2D) field effect transistors (FETs) with nanosecond scale switching speeds. In EDL gating, oppositely charged ions are accumulated near the 2D semiconductor surface, which induce image charges in the channel. This approach yields large capacitance densities corresponding to sheet carrier densities on the order of 1013 -1014 cm-2. The monolayer electrolyte random access memory (i.e., MERAM) consists of cobalt crown ether phthalocyanine (CoCrPc) and lithium ions deposited as a monolayer on the surface a 2D semiconductor (WSe2) by drop casting and annealing. CoCrPc is an electrically insulating (band gap ~ 1.34 eV) material with four crown ethers and it lays flat on the surface of a 2D semiconductor. Each crown solvates a Li+ ion that can diffuse up or down through the crown ether cavity. In response to an applied electric field, Li+ ions diffuse through the crown ether cavity and are positioned either near or away from the channel resulting in on and off states, respectively. We have previously shown switching behavior on 2D FETs using this material with potential application in non-volatile memory. Achieving well-ordered monolayers of CoCrPc and complete solvation of Li+ into the crown ethers are critical for device operation because the location and orientation of the molecules governs the device mechanism. When the well-ordered electrolyte layer deposited on a WSe2 FET is capped with h-BN, the off-state is stabilized (as confirmed by density functional theory (DFT)) by providing an energetically favorable state to Li+ ions. We have demonstrated the bistability using back-gated pulsed voltage testing with pulse width of 1 sec (± 30 V). Switching speeds down to 50 nanoseconds (limit of the instrument) are demonstrated with an on-off current ratio > 103. Further, we performed the endurance test on the device and demonstrated the stability of the device for 1000 cycles (max. measured) with 50 ns pulse. The on-off current ratio was maintained (> 103) even after 1000 switching cycles. Current work includes quantifying performance metrics for several devices and top-gating these devices to decrease program/erase voltages.

High-Speed Two-Dimensional Solid-State Non-Volatile Memory Based on Electric Double Layer Gating Using a Monolayer Electrolyte

Abstract Body: Nanowire light-emitting diodes (LEDs) have long been investigated as alternatives to conventional mesa LEDs, as they allow for increased light extraction efficiency (LEE) and a reduction of the internal electric field strength in AlInGaN alloys. Nanowires also show potential for use as single pixels in micro-LED (µLED) displays and photonic crystal surface-emitting laser diodes (PCSELs). While epitaxially grown nanowires allow for higher material quality in the active region and reduction of the quantum confined Stark effect, they often suffer from uniformity and yield issues, and are difficult to fabricate into ordered, addressable arrays. Nanowires can alternatively be formed through dry-etching of epitaxially grown light emitting layers, taking advantage of processes and tools developed by the semiconductor industry. The general process for fabricating a nanowire array LED involves dry-etching of an n-i-p epitaxial stack to form high aspect ratio structures, followed by deposition of the n-contact metal, application of an interlayer dielectric, and deposition of the p-contact material. As most LEDs emitting in the visible range are based on the AlInGaN material system, an aggressive Cl2 plasma must be used to perform the dry-etch. The poor selectivity of Cl2 plasmas against conventional dry-etch hardmask materials such as photoresist and SiO2 necessitates the use of a metal hardmask such as Ni, which is capable of withstanding the extended etch times required to form nanowires with heights greater than 1 µm. This thick Ni hardmask must be removed from the nanowires in order to maximize LEE. In devices which use self-masked n-metal deposition, in which the nanowires themselves act at the mask for deposition of a universal n-contact, wet etching of the Ni hardmask following deposition of the n-metal (which itself often contains Ni) is not possible, because the chemistries commonly used to etch Ni will also attack the other metals in the n-metal stack (Ti, Al, Ni, etc.). For this reason, an alternative method of removing the Ni hardmask is desired. In this work, we present a novel method for removing a metal hardmask from the tops of dry-etched GaN nanowires which does not involve metal etch chemistry, but instead relies upon an underlying “liftoff” layer to separate a thick metal “cap” from the tops of the nanowires. A 300 nm layer of SiO2 is deposited on the wafer, followed by patterning of the Ni hardmask through a liftoff process. The Ni is then used to mask a CF4/CHF3 dry-etch of the underlying SiO2, and a subsequent Cl2/Ar dry-etch of the GaN, with ~200 nm of Ni capable of withstanding etch depths of more than 7 µm. The nanowires are then etched in a KOH solution to remove dry-etch damage and smooth the sidewalls of the nanowires. A universal n-metal (Ti/Al/Ni/Ag) contact, masked by the nanowires themselves, is then deposited and annealed. A buffered oxide etch (BOE) solution is then used to remove the SiO2 layer, releasing the thick metal caps (Ni/Ti/Al/Ni/Ag) which are washed away in the etch solution. Polydimethylsiloxane (PDMS) is then coated over the “bare” nanowires and etch-back to expose the p-GaN nanowire tips. A transparent top contact, either ITO or thin (<20 nm) Ni is then deposited, making contact to the tops of the nanowires and linking many of them in series, allowing for electrical excitation of arbitrarily large arrays simultaneously. Using this process, we have fabricated high brightness arrays of 2.5 µm diameter electrically driven nanowires emitting at 550 nm with a linewidth of ~40 nm. Removal of the metal cap from the nanowires allows for increased LEE from extremely uniform arrays, while the use of a universal n-metal contact allows for decreased series resistance and more uniform emission intensity from larger arrays. This novel fabrication approach can allow for more efficient top-down fabricated light-emitting nanowire arrays, which are of interest for use in LEDs, µLED displays, and PCSELs.

Realization of High-Efficiency Green InGaN Nanowire Light-Emitting Diodes Using a Novel Dry-Etch Hardmask Removal Process

Abstract Body: Organic photovoltaics (OPVs) based on nonfullerene small molecule acceptors have been the subject of renewable energy research in the past five years. Ternary photovoltaic blends comprising a polymer donor, a nonfullerene small molecule acceptor, and a fullerene acceptor have proved to be most efficient active layers for OPV devices. However, the morphological parameters and their relations with mechanical properties and photovoltaic performance of this type of highly efficient polymer:nonfullerene:fullerene OPVs are still unknown to date. To address this question, we characterized the thin-film microstructure and mechanical behavior of the best-performing ternary OPV active layer (PM6:N3:PC71BM). Specifically, we alter the relative weight ratio of acceptors and systematically examined the composition dependence of photovoltaic performance, surface/bulk morphology, and mechanical parameters of the ternary blend films. It is shown that the addition of 20 wt% PC71BM to the acceptor component results in the highest power conversion efficiency (PCE) and crack-onset strain (COS) (Figure 1a). Most notably, we discover that it is possible to predict the elastic modulus of the ternary blend films by an extended Halpin-Tsai model (Figure 1b). This work provides simple guidelines for predicting the mechanical properties of many electronic devices based on ternary blends.

Manipulation of Morphological, Mechanical and Photovoltaic Properties of Ternary Organic Photovoltaic Blends for Optimum Operation

Abstract Body: Metal halide perovskites (MHPs) have rapidly become a topic of intense interest in both materials physics and device engineering due to their much sought for properties like high charge carrier mobilities, tunable bandgap, and low-cost processability. Various high-performance devices based on MHPs, including photovoltaic cells, light-emitting diodes, transistors and photodetectors have been reported, but a thorough understanding of the mechanism of charge transport and photo-transport in this material is still lacking. Here, we explore the photocurrent properties in bilayers consisting of small molecule organic semiconductors (OSCs) and MHPs. The MHP CH3NH3PbI3-xClx was the primary photoactive layer and electron transport layer, while the OSC hole transport layer was 2,8-Difluoro-6,13-Bis(triisopropylsilylethynyl) anthradithiophene (diF-TIPS-ADT). We found that the responsivity of the bilayer optimized device was 28 times greater than neat perovskite film, reaching values as high as 6.4 A/W. Detectivity also improved by a factor of 9, to 1.4*1011 Jones, in devices with optimum film morphology. We found that the photoresponse can be tuned by altering the microstructure of the organic semiconductor: treatment of the device contacts with (2,3,4,5,6)-Pentafluorothiophenol (PFBT) resulted in grains as large as 155 µm2 (LG) within the OSC, compared to much smaller grains (SG) seen when the OSC was deposited on the bare Au contacts, which resulted in grains in the order of 10 - 15 µm2. Additionally, in the heterostructure devices made on a large grain OSC film, hysteresis was eliminated. X-ray diffraction measurements indicate that the crystal structure of both the OSC and MHP is similar in all samples, with diF-TIPS-ADT preferentially oriented with its (001) plane parallel to the substrate, and MHP adopting its tetragonal phase. We concluded that the observed performance improvement does not originate from differences in the interfacial coupling related to molecular orientation or differences in MHP crystal phase. Instead, we conclude that reducing charge trapping at grain boundaries within the OSC layer extends photocarrier lifetime, leading to an improvement in performance.

Current Noise Analysis on Organo-Metal Halide Perovskite Resistive Switching Memory

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Composition and Electrical Characterization of ScxAl1-xN Grown on Si Substrate by DC Sputtering

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