Area-selective atomic layer deposition on 2D monolayer lateral superlattices.

The advanced patterning process is the basis of integration technology to realize the development of next-generation high-speed, low-power consumption devices. Recently, area-selective atomic layer deposition (AS-ALD), which allows the direct deposition of target materials on the desired area using a deposition barrier, has emerged as an alternative patterning process. However, the AS-ALD process remains challenging to use for the improvement of patterning resolution and selectivity. In this study, we report a superlattice-based AS-ALD (SAS-ALD) process using a two-dimensional (2D) MoS2-MoSe2 lateral superlattice as a pre-defining template. We achieved a minimum half pitch size of a sub-10 nm scale for the resulting AS-ALD on the 2D superlattice template by controlling the duration time of chemical vapor deposition (CVD) precursors. SAS-ALD introduces a mechanism that enables selectivity through the adsorption and diffusion processes of ALD precursors, distinctly different from conventional AS-ALD method. This technique facilitates selective deposition even on small pattern sizes and is compatible with the use of highly reactive precursors like trimethyl aluminum. Moreover, it allows for the selective deposition of a variety of materials, including Al2O3, HfO2, Ru, Te, and Sb2Se3.

Layer-Controlled Growth of Single-Crystalline 2D Bi2O2Se Film Driven by Interfacial Reconstruction.

As semiconductor scaling continues to reach sub-nanometer levels, two-dimensional (2D) semiconductors are emerging as a promising candidate for the post-silicon material. Among these alternatives, Bi2O2Se has risen as an exceptionally promising 2D semiconductor thanks to its excellent electrical properties, attributed to its appropriate bandgap and small effective mass. However, unlike other 2D materials, growth of large-scale Bi2O2Se films with precise layer control is still challenging due to its large surface energy caused by relatively strong interlayer electrostatic interactions. Here, we present the successful growth of a wafer-scale (∼3 cm) Bi2O2Se film with precise thickness control down to the monolayer level on TiO2-terminated SrTiO3 using metal-organic chemical vapor deposition (MOCVD). Scanning transmission electron microscopy (STEM) analysis confirmed the formation of a [BiTiO4]1- interfacial structure, and density functional theory (DFT) calculations revealed that the formation of [BiTiO4]1- significantly reduced the interfacial energy between Bi2O2Se and SrTiO3, thereby promoting 2D growth. Additionally, spectral responsivity measurements of two-terminal devices confirmed a bandgap increase of up to 1.9 eV in monolayer Bi2O2Se, which is consistent with our DFT calculations. Finally, we demonstrated high-performance Bi2O2Se field-effect transistor (FET) arrays, exhibiting an excellent average electron mobility of 56.29 cm2/(V·s). This process is anticipated to enable wafer-scale applications of 2D Bi2O2Se and facilitate exploration of intriguing physical phenomena in confined 2D systems.

Indium-Gallium-Zinc Oxide-Based Synaptic Charge Trap Flash for Spiking Neural Network-Restricted Boltzmann Machine.

Recently, neuromorphic computing has been proposed to overcome the drawbacks of the current von Neumann computing architecture. Especially, spiking neural network (SNN) has received significant attention due to its ability to mimic the spike-driven behavior of biological neurons and synapses, potentially leading to low-power consumption and other advantages. In this work, we designed the indium-gallium-zinc oxide (IGZO) channel charge-trap flash (CTF) synaptic device based on a HfO2/Al2O3/Si3N4/Al2O3 layer. Our IGZO-based CTF device exhibits synaptic functions with 128 levels of synaptic weight states and spike-timing-dependent plasticity. The SNN-restricted Boltzmann machine was used to simulate the fabricated CTF device to evaluate the efficiency for the SNN system, achieving the high pattern-recognition accuracy of 83.9%. We believe that our results show the suitability of the fabricated IGZO CTF device as a synaptic device for neuromorphic computing.

Surface-Dominated HfO2 Nanorod-Based Memristor Exhibiting Highly Linear and Symmetrical Conductance Modulation for High-Precision Neuromorphic Computing.

The switching characteristics and performance of oxide-based memristors are predominately determined by oxygen- or oxygen-vacancy-mediated redox reactions and the consequent formation of conducting filaments (CFs). Devices using oxide thin films as the switching layer usually require an electroforming process for subsequent switching operations, which induces large device-to-device variations. In addition, the hard-to-control redox reaction during repeated switching causes random fluctuations or degradation of each resistance state, hindering reliable switching operations. In this study, an HfO2 nanorod (NR)-based memristor is proposed for simultaneously achieving highly uniform, electroforming-free, fast, and reliable analogue switching properties. The well-controlled redox reaction due to the easy gas exchange with the environment at the surface of the NRs enhances the generation of oxygen or oxygen vacancies during the switching operation, resulting in electroforming-free and reliable switching behavior. In addition, the one-dimensional surface growth of CFs facilitates highly linear conductance modulation with smaller conductance changes compared with the two-dimensional volume growth in thin-film-based memristors, resulting in a high accuracy of >92% in the Modified National Institute of Standards and Technology pattern-recognition test and desirable spike-timing-dependent plasticity.

Large Memory Window of van der Waals Heterostructure Devices Based on MOCVD-Grown 2D Layered Ge4 Se9.

Van der Waals (vdW) heterostructures have drawn much interest over the last decade owing to their absence of dangling bonds and their intriguing low-dimensional properties. The emergence of 2D materials has enabled the achievement of significant progress in both the discovery of physical phenomena and the realization of superior devices. In this work, the group IV metal chalcogenide 2D-layered Ge4 Se9 is introduced as a new selection of insulating vdW material. 2D-layered Ge4 Se9 is synthesized with a rectangular shape using the metalcorganic chemical vapor deposition system using a liquid germanium precursor at 240 °C. By stacking the Ge4 Se9 and MoS2 , vdW heterostructure devices are fabricated with a giant memory window of 129 V by sweeping back gate range of ±80 V. The gate-independent decay time reveals that the large hysteresis is induced by the interfacial charge transfer, which originates from the low band offset. Moreover, repeatable conductance changes are observed over the 2250 pulses with low non-linearity values of 0.26 and 0.95 for potentiation and depression curves, respectively. The energy consumption of the MoS2 /Ge4 Se9 device is about 15 fJ for operating energy and the learning accuracy of image classification reaches 88.3%, which further proves the great potential of artificial synapses.

Gas-Phase Alkali Metal-Assisted MOCVD Growth of 2D Transition Metal Dichalcogenides for Large-Scale Precise Nucleation Control.

Advances in large-area and high-quality 2D transition metal dichalcogenides (TMDCs) growth are essential for semiconductor applications. Here, the gas-phase alkali metal-assisted metal-organic chemical vapor deposition (GAA-MOCVD) of 2D TMDCs is reported. It is determined that sodium propionate (SP) is an ideal gas-phase alkali-metal additive for nucleation control in the MOCVD of 2D TMDCs. The grain size of MoS2 in the GAA-MOCVD process is larger than that in the conventional MOCVD process. This method can be applied to the growth of various TMDCs (MoS2 , MoSe2 , WSe2 , and WSe2 ) and the generation of large-scale continuous films. Furthermore, the growth behaviors of MoS2 under different SP and oxygen injection time conditions are systematically investigated to determine the effects of SP and oxygen on nucleation control in the GAA-MOCVD process. It is found that the combination of SP and oxygen increases the grain size and nucleation suppression of MoS2 . Thus, the GAA-MOCVD with a precise and controllable supply of a gas-phase alkali metal and oxygen allows achievement of optimum growth conditions that maximizes the grain size of MoS2 . It is expected that GAA-MOCVD can provide a way for batch fabrication of large-scale atomically thin electronic devices based on 2D semiconductors.

Growth and Interlayer Engineering of 2D Layered Semiconductors for Future Electronics.

Layered materials that do not form a covalent bond in a vertical direction can be prepared in a few atoms to one atom thickness without dangling bonds. This distinctive characteristic of limiting thickness around the sub-nanometer level allowed scientists to explore various physical phenomena in the quantum realm. In addition to the contribution to fundamental science, various applications were proposed. Representatively, they were suggested as a promising material for future electronics. This is because (i) the dangling-bond-free nature inhibits surface scattering, thus carrier mobility can be maintained at sub-nanometer range; (ii) the ultrathin nature allows the short-channel effect to be overcome. In order to establish fundamental discoveries and utilize them in practical applications, appropriate preparation methods are required. On the other hand, adjusting properties to fit the desired application properly is another critical issue. Hence, in this review, we first describe the preparation method of layered materials. Proper growth techniques for target applications and the growth of emerging materials at the beginning stage will be extensively discussed. In addition, we suggest interlayer engineering via intercalation as a method for the development of artificial crystal. Since infinite combinations of the host-intercalant combination are possible, it is expected to expand the material system from the current compound system. Finally, inevitable factors that layered materials must face to be used as electronic applications will be introduced with possible solutions. Emerging electronic devices realized by layered materials are also discussed.

Polarization and Localization of Single-Photon Emitters in Hexagonal Boron Nitride Wrinkles.

Color centers in two-dimensional hexagonal boron nitride (h-BN) have recently emerged as stable and bright single-photon emitters (SPEs) operating at room temperature. In this study, we combine theory and experiment to show that vacancy-based SPEs selectively form at nanoscale wrinkles in h-BN with its optical dipole preferentially aligned to the wrinkle direction. By using density functional theory calculations, we find that the wrinkle's curvature plays a crucial role in localizing vacancy-based SPE candidates and aligning the defect's symmetry plane to the wrinkle direction. By performing optical measurements on SPEs created in h-BN single-crystal flakes, we experimentally confirm the wrinkle-induced generation of SPEs and their polarization alignment to the wrinkle direction. Our results not only provide a new route to controlling the atomic position and the optical property of the SPEs but also revealed the possible crystallographic origin of the SPEs in h-BN, greatly enhancing their potential for use in solid-state quantum photonics and quantum information processing.

Position and Frequency Control of Strain-Induced Quantum Emitters in WSe2 Monolayers.

Future scalable and integrated quantum photonic systems require deterministic generation and control of multiple quantum emitters. Although various approaches for spatial and spectral control of the quantum emitters have been developed, on-chip control of both position and frequency is still a long-standing goal in solid-state quantum emitters. Here, we demonstrate simultaneous control of position and frequency of the quantum emitters from transition metal dichalcogenide monolayers. Atomically thin two-dimensional materials are inherently sensitive to external strain and offer a new opportunity of creating and controlling the quantum emitters by engineering strain. We fabricate an electrostatically actuated microcantilever with nanopyramid patterns, providing a local strain engineering platform for the WSe2 monolayer. The integrated WSe2 generates high-purity single photon emission at patterned positions with a tuning range up to 3.5 meV. Together with the position and frequency control, we investigate the strain response on the fine-structure splitting and confirm 11% reduction in the fine splitting at the estimated tensile strain of 0.07%.

Stark Tuning of Single-Photon Emitters in Hexagonal Boron Nitride.

Single-photon emitters play an essential role in quantum technologies, including quantum computing and quantum communications. Atomic defects in hexagonal boron nitride ( h-BN) have recently emerged as new room-temperature single-photon emitters in solid-state systems, but the development of scalable and tunable h-BN single-photon emitters requires external methods that can control the emission energy of individual defects. Here, by fabricating van der Waals heterostructures of h-BN and graphene, we demonstrate the electrical control of single-photon emission from atomic defects in h-BN via the Stark effect. By applying an out-of-plane electric field through graphene gates, we observed Stark shifts as large as 5.4 nm per GV/m. The Stark shift generated upon a vertical electric field suggests the existence of out-of-plane dipole moments associated with atomic defect emitters, which is supported by first-principles theoretical calculations. Furthermore, we found field-induced discrete modification and stabilization of emission intensity, which were reversibly controllable with an external electric field.