Nonvolatile Memory Devices Research Articles

Near room temperature multilevel resistive switching memory with thin film ionic liquid crystals

Multilevel operation of nonvolatile resistive random-access memory devices was demonstrated using thin films of an ionic liquid crystal, 1-dodecyl-3-methylimidazolium tetrafluoroborate ([C12mim][BF4]), as a resistive switching layer.

Experimental demonstration of combination-encoding content-addressable memory of 0.75 bits per switch utilizing Hf-Zr-O ferroelectric tunnel junctions.

We experimentally demonstrate the concept of combination-encoding content-addressable memory (CECAM) that offers much higher content density than any other content-addressable memory devices proposed to date. In this work, CECAM was fabricated and validated with a hafnium-zirconium oxide (HZO) ferroelectric tunnel junction (FTJ) crossbar array. The new CAM structure, which utilizes nonvolatile memory devices, offers numerous advantages including low-current operation (FTJ), standby power reduction (ferroelectric HZO), and increased content density. Multibit data are encoded and stored in multi-switch CECAM. Perfect-match searching in CECAM with a reasonable match current (lower than nA) for different sizes of CECAM has been validated from a novel CAM device. We demonstrate N-CECAM (with keys encoded into 2N-long binary arrays) for N = 3 (using 6 FTJs) and 4 (using 8 FTJs), leading to content densities of 0.667 and 0.75 bits per switch, which highlight 33% and 50% increase in content density compared to that of the conventional TCAM (0.5 bits per switch).

Nanotube ferroelectric tunnel junctions with an ultrahigh tunneling electroresistance ratio.

Low-dimensional ferroelectric tunnel junctions are appealing for the realization of nanoscale nonvolatile memory devices due to their inherent advantages of device miniaturization. Those based on current mechanisms have limitations, including low tunneling electroresistance (TER) effects and complex heterostructures. Here, we introduce an entirely new TER mechanism to construct a nanotube ferroelectric tunnel junction with ferroelectric nanotubes as the tunneling region. When rolling a ferroelectric monolayer into a nanotube, due to the coexistence of its intrinsic ferroelectric polarization with the flexoelectric polarization induced by bending, a metal-insulator transition occurs depending on the radiative polarization states. For the pristine monolayer, its out-of-plane polarization is tunable by an in-plane electric field, and the conducting states of the ferroelectric nanotube can thus be tuned between metallic and insulating states via axial electric means. Using α-In2Se3 as an example, our first-principles density functional theory calculations and nonequilibrium Green's function formalism confirm the feasibility of the TER mechanism and indicate an ultrahigh TER ratio that exceeds 9.9 × 1010% of the proposed nanotube ferroelectric tunnel junctions. Our findings provide a promising approach based on simple homogeneous structures for high density ferroelectric microelectric devices with excellent ON/OFF performance.

Thermally-induced nanoscale phase change in chalcogenide glass Cr2Ge2Te6 revealed by scanning tunneling microscopy

Cr2Ge2Te6 (CrGT) is viewed as an important phase change material (PCM) for next-generation nonvolatile memory devices because of its superior properties, e.g., high thermal stability and low operation energy, compared to conventional PCMs. However, the phase change mechanism of CrGT remains unsolved, especially at the nanoscale. Here, we investigated thermally induced nanoscale phase changes of CrGT thin films using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). By performing statistical analysis of the measured STM topographic and STS data, we evaluated the inhomogeneity and distribution of the phase change characteristics of CrGT thin films. We also related the nanoscale phase change properties of CrGT to macroscopic phase changes by comparing the STM and STS results with experimental data from Raman spectroscopy.

High tunneling electroresistance in ferroelectric tunnel junctions based on two-dimensional α-In2Se3/MoTe2 van der Waals heterostructures.

Ferroelectric polarization-controlled band alignment can be realized in van der Waals heterostructures (vdWHs), which can be used to create new types of ferroelectric tunnel junctions (FTJs). In this work, we design six probable configurations of two-dimensional vdWHs based on a two-dimensional α-In2Se3 ferroelectric material which has two opposite polarization states P↑ and P↓, and the semiconductor MoTe2. First-principles calculations show robust ferroelectric polarization-controlled switching behavior between the high conductance state in configuration AA-P↓ and the low conductance state in configuration AA-P↑ in the most stable AA stacked vdWHs. Based on this vdWH, a two-dimensional transverse FTJ with AA-P↓ or AA-P↑ as the tunneling barrier and (In0.5Sn0.5)2Se3 monolayers (n-type doped) as electrodes is designed. The tunneling electroresistance ratio of the FTJs at the Fermi level reaches 1.22 × 104% when the tunneling barrier contains two repeating units N = 2 and can be greatly increased by increasing the thickness of the ferroelectric layer. Analysis of the work function, charge redistribution, and local density of states is performed to interpret the above phenomena. The findings suggest the great potential of the AA stacked α-In2Se3/MoTe2 vdWH in the design of high-performance FTJs and application in high-density non-volatile memory devices.

Kinetic Monte Carlo simulations on electroforming in nanomanipulated conductive bridge random access memory devices.

Conductive bridge random access memory (CBRAM) devices exhibit great potential as the next-generation nonvolatile memory devices. However, they suffer from two major disadvantages, namely relatively high power consumption and large cycle-to-cycle and device-to-device variations, which hinder their more extensive commercialization. To learn how to enhance their device performance, kinetic Monte Carlo (KMC) simulations were employed to illustrate the variation of electroforming processes in nanomanipulated CBRAM devices by introducing an ion-blocking layer with scalable nanopores and tuning the microstructures of dielectric layers. Both the size of nanopores and the inhomogeneity of dielectric layers have significant impacts on the forming processes of conductive filaments. The dielectric layer with a high-content loose texture plus the scalable nanopore-containing ion-blocking layer leads to the formation of size-controlled and uniform filaments, which remarkably contributes to miniaturizable and stable CBRAM devices. Our study provides insights into nanomanipulation strategies to realize high-performance CBRAM devices, still awaiting future experimental confirmation.

Optical and structural characterizations of NiO-doped PMMA films and fabrication of Ag/NiO-doped PMMA/n-Si/AuSb for analogue-digital switching applications

Herein, the authors report the NiO-doped PMMA nanocomposites fabrication process with different Ni concentrations of 0.001–10 wt% on pre-cleaned glass, ITO, and n-type Si via spin-coating technique. X-ray diffraction (XRD) was used to analyze the crystal structure of NiO in powder form and the NiO-doped PMMA nanocomposite thin films. The Rietveld refinement method was used to analyze the manufactured NiO's powder-form structural characteristics. The analysis data revealed a single phase of NiO nanoparticles with face-centred cubic of Fm-3m space group. The average crystallites' mean size and the microstrain value were determined based on the Williamson-Hall model and were equal to 32.47 ± 1.210 nm and 5 × 10−5, respectively. The FESEM micrographs illustrate dispersed cubic-shaped NiO grains in the PMMA matrix. The estimated energy gaps and the width of the localized energy states (Urbach tails) are plotted against the photon energy. The estimated energy gap, EgOp is increasing from 3.649 ± 0.003 eV to 3.782 ± 0.005 eV with increasing the NiO nanoparticles' doping ratio in the PMMA as a host insulating polymer. The fabricated Ag/NiO-PMMA (S4)/n-Si/AuSb heterojunction device revealed two different (HRS and LRS) resistance-switching behaviours. For second and third electrical (I–V) paths, the extracted magnitudes of the ideality factor are 2.397 ± 0.006 and 2.691 ± 0.003 and the calculated barrier height are 0.727 ± 0.004 and 0.886 ± 0.005, respectively. The interfacial electronics states NSS increasing from 6.58 × 1012 to 3.7 × 1014 cm−2.eV−1 and 3.48 × 1013 to 3.65 × 1014 cm−2 .eV−1 for the 2nd HRS path and 3rd LRS, respectively. The investigated hysteresis loop and the variation in interfacial electronics states reveal that the NiO-PMMA nanocomposite may be promising in non-volatile memory and electrical switching electronic devices.

Magneto-electric coupling beyond van der Waals interaction in two-dimensional multiferroic heterostructures

Exploring two-dimensional (2D) multiferroic systems with strong magneto-electric coupling properties holds significant application value in nanoscale spintronics devices. However, due to the weak interlayer van der Waals interactions, strong magneto-electric coupling in 2D heterostructures is relatively rare. By using first-principles simulations, we demonstrate that in the NiPS3/Sc2CO2 heterostructure, the ferroelectric polarization switching of the Sc2CO2 layer induces a transition in the magnetic ground state of the NiPS3 layer from the ferromagnetic state to antiferromagnetic ordering, accompanied by a transformation from a semiconductor to a half-metallic state. This magnetic phase transition is caused by a novel magneto-electric coupling mechanism: the polarization switching changes the band alignment between the two materials and then induces a significant interlayer charge transfer, leading to the emergence of Stoner itinerant ferromagnetism. In addition, the polarization switching can also change the magnetic anisotropy from an easy magnetization plane to an easy magnetization axis. These results not only offer a promising multiferroic heterostructure for nonvolatile memory devices and magnetic sensors but also provide a feasible approach for designing multiferroic system with strong magneto-electric coupling.

(Invited) Fabrication Technique of Ferroelectric HfxZr1−XO2 Thin Films Using ALD-ZrO2 Nucleation Layers

Ferroelectric HfxZr1−xO2 (HZO) thin films have attracted considerable attention towards high-density and low-power ferroelectric memory devices of ferroelectric random access memory (FeRAM) and ferroelectric field-effect transistors (FeFETs) [1]. To obtain ferroelectric orthorhombic (O) phase of HZO films, several techniques have been investigated, such as the TiN stressor layer technique [2] and controlled annealing conditions [3]. On the other hand, we pay attention to the ZrO2 nucleation layer technique because ZrO2 films deposited by atomic layer deposition (ALD) method formed a nanocrystalline structure and consisted dominantly of O, tetragonal (T), and cubic (C) phases, whose lattice constants are considerably close to that of ferroelectric O phase for HfO2 [4]. In this paper, we report the crystallinity and ferroelectricity of HZO films fabricated using the ZrO2 nucleation layer technique for metal-ferroelectric-metal (MFM) and metal-ferroelectric-semiconductor (MFS) capacitors.First, four types of MFM capacitors of TiN/HZO/TiN (MFM w/o), TiN/HZO/bottom-ZrO2/TiN (MFM B-ZrO2), TiN/top-ZrO2/HZO/TiN (MFM T-ZrO2), and TiN/top-ZrO2/HZO/bottom-ZrO2/TiN (MFM D-ZrO2) were systematically investigated for the FeRAM applications [5]. The thicknesses of the ALD-grown HZO and ZrO2 films were 10 and 2 nm, respectively. The post-deposition annealing was performed at 600°C. The remanent polarization (2P r = P r + − P r −) of the MFM capacitors increased in the following order: MFM w/o (12 µC/cm2) < MFM B-ZrO2 (15 µC/cm2) < MFM T-ZrO2 (23 µC/cm2) < MFM D-ZrO2 (29 µC/cm2), while all capacitors showed almost the same coercive electric field (E c) value of around 1.2 MV/cm. Therefore, maximum 2P rvalue of the MFM capacitor was obtained using the top- and bottom-ZrO2 nucleation layers. For the MFM capacitors with ZrO2 nucleation layers, epitaxial-like grain growth of the HZO film occurred on the nanocrystalline top- and bottom-ZrO2 layers. Moreover, the relative ratio of O/T/C phases in the ferroelectric film, which was estimated using the peak area ratio of O(111)/T(101)/C(111)/{M(−111)+ O(111)/T(101)/C(111)+M(111)}, increased in the following order: MFM w/o < MFM B-ZrO2 < MFM T-ZrO2 < MFM D-ZrO2. Therefore, the top- and bottom-ZrO2 layers play an important role as nucleation layers for the crystallization of the HZO film, resulting in a larger relative ratio of O/T/C phases in the ferroelectric film compared to w/o. Moreover, these results indicate that the top-ZrO2 layer was more effective to form the ferroelectric phase compared to the bottom-ZrO2 layer.Next, two types of MFS capacitors of TiN/HZO/Si (MFS w/o) and TiN/top-ZrO2/HZO/Si (MFS T-ZrO2) were fabricated by low-temperature processes at 300°C of ALD and post-metallization annealing (PMA) for the FeFET applications [6]. The thicknesses of both HZO and ZrO2 films were 10 nm. Both MFS w/o and MFS T-ZrO2 were found to form an extremely thin SiO2 interfacial layer with a thickness of one or two monolayers between the HZO film and Si substrate due to a low temperature fabrication process of 300°C. The HZO film of the MFS T-ZrO2 formed O/T/C phases even with a low thermal budget of 300°C, while that of the MFS w/o had an amorphous structure. This result is attributed to the beneficial role of the nanocrystalline top-ZrO2 nucleation layer for the crystallization of an amorphous HZO film during the PMA process. Therefore, a higher 2P r value of 15 µC/cm2 was obtained for the MFS T-ZrO2 than that (2.2 µC/cm2) for the MFS w/o. Moreover, the endurance properties of the MFS T-ZrO2 were free from the wake-up effect and exhibited less degradation of switching polarization (P sw). This could be attributed to the insertion of a ZrO2 film at the TiN/HZO interface, which promoted the preferential formation of the ferroelectric orthorhombic phase and prevent the formation of oxygen vacancies at the ZrO2/HZO interface. Thus, we concluded that superior ferroelectricity with wake-up free properties and higher fatigue resistance of HZO-based MFS capacitors were achieved by using the ZrO2 nucleation layer technique.These results suggest that the fabrication technique of ferroelectric HZO films using nanocrystalline ALD-ZrO2 nucleation layers is one of the promising processes for the next-generation non-volatile memory device applications.This work was supported by JSPS KAKENHI (Nos. JP21J01667, JP20H02189, and JP18J22998) and MEXT Leading Initiative for Excellent Young Researchers (No. JPMXS0320220213).[1] T. Mikolajick et al., J. Appl. Phys. 129, 100901 (2021).[2] S. J. Kim, et al., Appl. Phys. Lett. 111, 242901 (2017).[3] S. Migita et al., Jpn. J. Appl. Phys. 58, SBBA07 (2019).[4] T. Onaya et. al., Appl. Phys. Express. 10, 081501 (2017).[5] T. Onaya et al., APL Mater. 7, 061107 (2019).[6] T. Onaya et al., APL Mater. 10, 051110 (2022).

Phase-Change Memory from Molecular Tellurides.

Phase-change memory (PCM) is an emerging memory technology based on the resistance contrast between the crystalline and amorphous states of a material. Further development and realization of PCM as a mainstream memory technology rely on innovative materials and inexpensive fabrication methods. Here, we propose a generalizable and scalable solution-processing approach to synthesize phase-change telluride inks in order to meet demands for high-throughput material screening, increased energy efficiency, and advanced device architectures. Bulk tellurides, such as Sb2Te3, GeTe, Sc2Te3, and TiTe2, are dissolved and purified to obtain inks of molecular metal telluride complexes. This allowed us to unlock a wide range of solution-processed ternary tellurides by the simple mixing of binary inks. We demonstrate accurate and quantitative composition control, including prototype materials (Ge-Sb-Te) and emerging rare-earth-metal telluride-doped materials (Sc-Sb-Te). Spin-coating and annealing convert ink formulations into high-quality, phase-pure telluride films with preferred orientation along the (00l) direction. Deposition engineering of liquid tellurides enables thickness-tunable films, infilling of nanoscale vias, and film preparation on flexible substrates. Finally, we demonstrate cyclable and non-volatile prototype memory devices, achieving performance indicators such as resistance contrast and low reset energy on par with state-of-the-art sputtered PCM layers.

Highly Efficient Spin-Orbit Torque Switching in Bi2Se3/Fe3GeTe2 van der Waals Heterostructures.

Topological insulators (TIs) have shown promise as a spin-generating layer to switch the magnetization state of ferromagnets via spin-orbit torque (SOT) due to charge-to-spin conversion efficiency of the TI surface states that arises from spin-momentum locking. However, when TIs are interfaced with conventional bulk ferromagnetic metals, the combination of charge transfer and hybridization can potentially destroy the spin texture and hamper the possibility of accessing the TI surface states. Here, we fabricate an all van der Waals (vdW) heterostructure consisting of molecular beam epitaxy grown bulk-insulating Bi2Se3 and exfoliated 2D metallic ferromagnet Fe3GeTe2 (FGT) with perpendicular anisotropy. By detecting the magnetization state of the FGT via anomalous Hall effect and magneto-optical Kerr effect measurements, we determine the critical switching current density for magnetization switching to be Jc ≈ 1.2 × 106 A/cm2, the lowest reported for the switching of a perpendicular anisotropy ferromagnet using Bi2Se3. From second harmonic Hall measurements, we further determine the SOT efficiency (ξDL) to be in the range of 1.8 ± 0.3 and 1.4 ± 0.08 between 5 and 150 K, comparable to the highest values reported for Bi2Se3. Our density functional theory calculations find that the weak interlayer interactions at the Bi2Se3/FGT interface lead to a weakened dipole at the interface and suppress the proximity induced magnetic moment on Bi2Se3. This enables direct access to the TI surface states contributed by the first quintuple layer, where the spins are singly degenerate with significant net in-plane spin polarization. Our results highlight the clear advantage of all-vdW heterostructures with weak interlayer interactions that can enhance SOT efficiency and minimize critical current density, an important step toward realizing next generation low-power nonvolatile memory and spintronic devices.

Exploitable magnetic anisotropy and half-metallicity controls in multiferroic van der Waals heterostructure

Two-dimensional (2D) XY ferromagnets have drawn pronounced interest in recent years, but the characteristic of easy-plane magnetization restricts their application in spintronics to some extent. Here, we propose a general strategy for constructing multiferroic van der Waals heterostructures, aiming to achieve electrical control over the magnetic anisotropy in 2D XY ferromagnets. The validity of this strategy is verified by the heterostructure composed of ferromagnetic VBi2Te4 and ferroelectric In2Se3 monolayers. By manipulating the polarized states of In2Se3, the VBi2Te4 can be reversibly transformed between 2D XY and Heisenberg ferromagnets, characterized by the switching of easy magnetization axis between in-plane and out-of-plane directions. More interestingly, accompanied by the changes in magnetic anisotropy, the VBi2Te4 also demonstrates a phase transition from a semiconductor to a half-metal state, which can be ascribed to the band alignment and interfacial charge transfer. The switchable magnetic and electronic properties enable the heterostructure to be utilized in nonvolatile memory and logic devices. Additionally, the half-metallicity and magnetocrystalline anisotropy energy of the heterostructure can be effectively tuned by biaxial strain. These findings not only pave the way for electrically nonvolatile control of 2D XY ferromagnet, but also facilitate the development of interfacial magnetoelectric physics and applications.

In-memory analog solution of compressed sensing recovery in one step

Modern analog computing, by gaining momentum from nonvolatile resistive memory devices, deals with matrix computations. In-memory analog computing has been demonstrated for solving some basic but ordinary matrix problems in one step. Among the more complicated matrix problems, compressed sensing (CS) is a prominent example, whose recovery algorithms feature high-order matrix operations and hardware-unfriendly nonlinear functions. In light of the local competitive algorithm (LCA), here, we present a closed-loop, continuous-time resistive memory circuit for solving CS recovery in one step. Recovery of one-dimensional (1D) sparse signal and 2D compressive images has been experimentally demonstrated, showing elapsed times around few microseconds and normalized mean squared errors of 10 −2 . The LCA circuit is one or two orders of magnitude faster than conventional digital approaches. It also substantially outperforms other (electronic or exotically photonic) analog CS recovery methods in terms of speed, energy, and fidelity, thus representing a highly promising technology for real-time CS applications.

Flexible SnO2–MoS2 based memristive device exhibiting stable and enhanced memory phenomenon

Flexible non-volatile memory devices have been gaining interest in expanding the digital data storage world. Due to the burgeoning advancement in the healthcare industry, the Internet of Things, and wearable electronics, the demand for ultra-thin, low-power, and flexible memory is increasing. Further, the advancement of synthesis procedures for two-dimensional nanomaterials having better optical, electrical, and mechanical strength with flexibility has fuelled the flexible memory device area, as commonly used flash memory is approaching its physical limit. In this context, the present work reports the flexible resistive switching memory device based on pure molybdenum disulfide (MoS2) and tin oxide (SnO2) based nanocomposite powder synthesized using the simple hydrothermal process. The nanocomposite formation was characterized using x-ray diffraction and Raman spectroscopic techniques. The memory device was fabricated by spin-coating the pure MoS2, pure SnO2, and MoS2–SnO2 nanocomposite film over the ITO-PET flexible substrate. The device was completed by thermally evaporating the thin Al layer through a shadow mask. It was found that MoS2–SnO2 based memory devices exhibited improved switching performance having a higher I ON/I OFF ratio, and lower switching voltage in comparison to pure MoS2 and pure SnO2-based devices (I ON/I OFF ratio ∼100, V = 0.5 V). Furthermore, to check the stability and cyclic performance of the fabricated device, the retention and endurance test was also performed, and the MoS2–SnO2 device retained the HRS and LRS states up to 2 × 103s and showed stable performance up to 100 switching cycles without much degradation, respectively. It should be mentioned that the presently proposed ReRAM device based on SnO2 and MoS2 with flexible and low-power features had excellent potential for use in the wearable device industry.

Generalized Key-Value Memory to Flexibly Adjust Redundancy in Memory-Augmented Networks.

Memory-augmented neural networks enhance a neural network with an external key-value (KV) memory whose complexity is typically dominated by the number of support vectors in the key memory. We propose a generalized KV memory that decouples its dimension from the number of support vectors by introducing a free parameter that can arbitrarily add or remove redundancy to the key memory representation. In effect, it provides an additional degree of freedom to flexibly control the tradeoff between robustness and the resources required to store and compute the generalized KV memory. This is particularly useful for realizing the key memory on in-memory computing hardware where it exploits nonideal, but extremely efficient nonvolatile memory devices for dense storage and computation. Experimental results show that adapting this parameter on demand effectively mitigates up to 44% nonidealities, at equal accuracy and number of devices, without any need for neural network retraining.

High-performance van der Waals antiferroelectric CuCrP2S6-based memristors

Layered thio- and seleno-phosphate ferroelectrics, such as CuInP2S6, are promising building blocks for next-generation nonvolatile memory devices. However, because of the low Curie point, the CuInP2S6-based memory devices suffer from poor thermal stability (<42 °C). Here, exploiting the electric field-driven phase transition in the rarely studied antiferroelectric CuCrP2S6 crystals, we develop a nonvolatile memristor showing a sizable resistive-switching ratio of ~ 1000, high switching endurance up to 20,000 cycles, low cycle-to-cycle variation, and robust thermal stability up to 120 °C. The resistive switching is attributed to the ferroelectric polarization-modulated thermal emission accompanied by the Fowler–Nordheim tunneling across the interfaces. First-principles calculations reveal that the good device performances are associated with the exceptionally strong ferroelectric polarization in CuCrP2S6 crystal. Furthermore, the typical biological synaptic learning rules, such as long-term potentiation/depression and spike amplitude/spike time-dependent plasticity, are also demonstrated. The results highlight the great application potential of van der Waals antiferroelectrics in high-performance synaptic devices for neuromorphic computing.

Electron-Sponge Nature of Polyoxometalates for Next-Generation Electrocatalytic Water Splitting and Nonvolatile Neuromorphic Devices.

Designing next-generation molecular devices typically necessitates plentiful oxygen-bearing sites to facilitate multiple-electron transfers. However, the theoretical limits of existing materials for energy conversion and information storage devices make it inevitable to hunt for new competitors. Polyoxometalates (POMs), a unique class of metal-oxide clusters, have been investigated exponentially due to their structural diversity and tunable redox properties. POMs behave as electron-sponges owing to their intrinsic ability of reversible uptake-release of multiple electrons. In this review, numerous POM-frameworks together with desired features of a contender material and inherited properties of POMs are systematically discussed to demonstrate how and why the electron-sponge-like nature of POMs is beneficial to design next-generation water oxidation/reduction electrocatalysts, and neuromorphic nonvolatile resistance-switching random-access memory devices. The aim is to converge the attention of scientists who are working separately on electrocatalysts and memory devices, on a point that, although the application types are different, they all hunt for a material that could exhibit electron-sponge-like feature to realize boosted performances and thus, encouraging the scientists of two completely different fields to explore POMs as imperious contenders to design next-generation nanodevices. Finally, challenges and promising prospects in this research field are also highlighted.

Self‐assembled vapor-transport-deposited SnS nanoflake-based memory devices with synaptic learning properties

The most salient features of resistive switching (RS) devices are low energy consumption, fast switching speed, and high-density integration, which render them promising candidates for realizing non-volatile memory and artificial synaptic devices. However, the growth of functional switching layers for RS devices needs innovative deposition techniques. Herein, we utilize a high-throughput vapor-transport-deposition (VTD) technique for synthesizing self-assembled tin-sulfide (SnS) nanoflakes, which are then used as a switching layer to fabricate an RS device. First principle calculations are conducted to understand the optoelectronic properties of SnS by employing density functional theory. The proposed Ag/SnS/Pt memory device exhibits substantial merits, including low-switching voltages (VSET: 0.22 V and VRESET: −0.20 V), suitable ON/OFF ratio (∼259), excellent endurance (106), and extended memory retention (106 s) characteristics. In addition, RS stochasticity is modeled using statistical time-series analysis via Holt’s exponential smoothing. Interestingly, the device can emulate multiple synaptic functionalities, including potentiation, depression, paired-pulse facilitation, paired-pulse depression, excitatory postsynaptic current, inhibitory postsynaptic current, and advanced spike-timing dependent plasticity rules. Moreover, the proposed synaptic device can detect the edge of images by utilizing a convolutional neural network. The unique and efficient VTD-SnS-based device will be a potential candidate for high-density non-volatile memory and neuromorphic computing applications.

Out-of-plane ferroelectricity and robust magnetoelectricity in quasi-two-dimensional materials.

Thin-film ferroelectrics have been pursued for capacitive and nonvolatile memory devices. They rely on polarizations that are oriented in an out-of-plane direction to facilitate integration and addressability with complementary metal-oxide semiconductor architectures. The internal depolarization field, however, formed by surface charges can suppress the out-of-plane polarization in ultrathin ferroelectric films that could otherwise exhibit lower coercive fields and operate with lower power. Here, we unveil stabilization of a polar longitudinal optical (LO) mode in the n = 2 Ruddlesden-Popper family that produces out-of-plane ferroelectricity, persists under open-circuit boundary conditions, and is distinct from hyperferroelectricity. Our first-principles calculations show the stabilization of the LO mode is ubiquitous in chalcogenides and halides and relies on anharmonic trilinear mode coupling. We further show that the out-of-plane ferroelectricity can be predicted with a crystallographic tolerance factor, and we use these insights to design a room-temperature multiferroic with strong magnetoelectric coupling suitable for magneto-electric spin-orbit transistors.

Controlled Synthesis of Lead-Free Double Perovskite Colloidal Nanocrystals for Nonvolatile Resistive Memory Devices.

Although lead-free double perovskites such as Cs2AgBiBr6 have been widely explored, they still remain a daunting challenge for the controlled synthesis of lead-free double perovskite nanocrystals with highly tunable morphology and band structure. Here, we report the controlled synthesis of lead-free double perovskite colloidal nanocrystals including Cs2AgBiBr6 and Cs2AgInxBi1-xBr6 via a facile wet-chemical synthesis method for the fabrication of high-performance nonvolatile resistive memory devices. Cs2AgBiBr6 colloidal nanocrystals with well-defined cuboidal, hexagonal, and triangular morphologies are synthesized through a facile wet-chemical approach by tuning the reaction temperature from 150 to 190 °C. Further incorporating indium into Cs2AgBiBr6 to synthesize alloyed Cs2AgInxBi1-xBr6 nanocrystals not only can induce the indirect-to-direct bandgap transition with enhanced photoluminescence but also can improve its structural stability. After optimizing the active layers and device structure, the fabricated Ag/polymethylene acrylate@Cs2AgIn0.25Bi0.75Br6/ITO resistive memory device exhibits a low power consumption (the operating voltage is ∼0.17 V), excellent cycling stability (>10 000 cycles), and good synaptic property. Our study would enable the facile wet-chemical synthesis of lead-free double perovskite colloidal nanocrystals in a highly controllable manner for the development of high-performance resistive memory devices.