High energy density in artificial heterostructures through relaxation time modulation.

Electrostatic capacitors are foundational components of advanced electronics and high-power electrical systems owing to their ultrafast charging-discharging capability. Ferroelectric materials offer high maximum polarization, but high remnant polarization has hindered their effective deployment in energy storage applications. Previous methodologies have encountered problems because of the deteriorated crystallinity of the ferroelectric materials. We introduce an approach to control the relaxation time using two-dimensional (2D) materials while minimizing energy loss by using 2D/3D/2D heterostructures and preserving the crystallinity of ferroelectric 3D materials. Using this approach, we were able to achieve an energy density of 191.7 joules per cubic centimeter with an efficiency greater than 90%. This precise control over relaxation time holds promise for a wide array of applications and has the potential to accelerate the development of highly efficient energy storage systems.

Nondestructive Single-Atom-Thick Crystallographic Scanner via Sticky-Note-Like van der Waals Assembling-Disassembling.

Crystallographic characteristics, including grain boundaries and crystallographic orientation of each grain, are crucial in defining the properties of two-dimensional materials (2DMs). To date, local microstructure analysis of 2DMs, which requires destructive and complex processes, is primarily used to identify unknown 2DM specimens, hindering the subsequent use of characterized samples. Here, a nondestructive large-area 2D crystallographic analytical method through sticky-note-like van der Waals (vdW) assembling-disassembling is presented. By the vdW assembling of veiled polycrystalline graphene (PCG) with a single-atom-thick single-crystalline graphene filter (SCG-filter), detailed crystallographic information of each grain in PCGs is visualized through a 2D Raman signal scan, which relies on the interlayer twist angle. The scanned PCGs are seamlessly separated from the SCG-filter using vdW disassembling, preserving their original condition. The remaining SCG-filter is then reused for additional crystallographic scans of other PCGs. It is believed that the methods can pave the way for advances in the crystallographic analysis of single-atom-thick materials, offering huge implications for the applications of 2DMs.

Junctionless Negative-Differential-Resistance Device Using 2D Van-Der-Waals Layered Materials for Ternary Parallel Computing.

Negative-differential-resistance (NDR) devices offer a promising pathway for developing future computing technologies characterized by exceptionally low energy consumption, especially multivalued logic computing. Nevertheless, conventional approaches aimed at attaining the NDR phenomenon involve intricate junction configurations and/or external doping processes in the channel region, impeding the progress of NDR devices to the circuit and system levels. Here, an NDR device is presented that incorporates a channel without junctions. The NDR phenomenon is achieved by introducing a metal-insulator-semiconductor capacitor to a portion of the channel area. This approach establishes partial potential barrier and well that effectively restrict the movement of hole and electron carriers within specific voltage ranges. Consequently, this facilitates the implementation of both a ternary inverter and a ternary static-random-access-memory, which are essential components in the development of multivalued logic computing technology.

Monolithic 3D integration of 2D materials-based electronics towards ultimate edge computing solutions.

Three-dimensional (3D) hetero-integration technology is poised to revolutionize the field of electronics by stacking functional layers vertically, thereby creating novel 3D circuity architectures with high integration density and unparalleled multifunctionality. However, the conventional 3D integration technique involves complex wafer processing and intricate interlayer wiring. Here we demonstrate monolithic 3D integration of two-dimensional, material-based artificial intelligence (AI)-processing hardware with ultimate integrability and multifunctionality. A total of six layers of transistor and memristor arrays were vertically integrated into a 3D nanosystem to perform AI tasks, by peeling and stacking of AI processing layers made from bottom-up synthesized two-dimensional materials. This fully monolithic-3D-integrated AI system substantially reduces processing time, voltage drops, latency and footprint due to its densely packed AI processing layers with dense interlayer connectivity. The successful demonstration of this monolithic-3D-integrated AI system will not only provide a material-level solution for hetero-integration of electronics, but also pave the way for unprecedented multifunctional computing hardware with ultimate parallelism.

Functionalizing nanophotonic structures with 2D van der Waals materials.

The integration of two-dimensional (2D) van der Waals materials with nanostructures has triggered a wide spectrum of optical and optoelectronic applications. Photonic structures of conventional materials typically lack efficient reconfigurability or multifunctionality. Atomically thin 2D materials can thus generate new functionality and reconfigurability for a well-established library of photonic structures such as integrated waveguides, optical fibers, photonic crystals, and metasurfaces, to name a few. Meanwhile, the interaction between light and van der Waals materials can be drastically enhanced as well by leveraging micro-cavities or resonators with high optical confinement. The unique van der Waals surfaces of the 2D materials enable handiness in transfer and mixing with various prefabricated photonic templates with high degrees of freedom, functionalizing as the optical gain, modulation, sensing, or plasmonic media for diverse applications. Here, we review recent advances in synergizing 2D materials to nanophotonic structures for prototyping novel functionality or performance enhancements. Challenges in scalable 2D materials preparations and transfer, as well as emerging opportunities in integrating van der Waals building blocks beyond 2D materials are also discussed.

Applications of remote epitaxy and van der Waals epitaxy.

Epitaxy technology produces high-quality material building blocks that underpin various fields of applications. However, fundamental limitations exist for conventional epitaxy, such as the lattice matching constraints that have greatly narrowed down the choices of available epitaxial material combinations. Recent emerging epitaxy techniques such as remote and van der Waals epitaxy have shown exciting perspectives to overcome these limitations and provide freestanding nanomembranes for massive novel applications. Here, we review the mechanism and fundamentals for van der Waals and remote epitaxy to produce freestanding nanomembranes. Key benefits that are exclusive to these two growth strategies are comprehensively summarized. A number of original applications have also been discussed, highlighting the advantages of these freestanding films-based designs. Finally, we discuss the current limitations with possible solutions and potential future directions towards nanomembranes-based advanced heterogeneous integration.

High-throughput manufacturing of epitaxial membranes from a single wafer by 2D materials-based layer transfer process.

Layer transfer techniques have been extensively explored for semiconductor device fabrication as a path to reduce costs and to form heterogeneously integrated devices. These techniques entail isolating epitaxial layers from an expensive donor wafer to form freestanding membranes. However, current layer transfer processes are still low-throughput and too expensive to be commercially suitable. Here we report a high-throughput layer transfer technique that can produce multiple compound semiconductor membranes from a single wafer. We directly grow two-dimensional (2D) materials on III-N and III-V substrates using epitaxy tools, which enables a scheme comprised of multiple alternating layers of 2D materials and epilayers that can be formed by a single growth run. Each epilayer in the multistack structure is then harvested by layer-by-layer mechanical exfoliation, producing multiple freestanding membranes from a single wafer without involving time-consuming processes such as sacrificial layer etching or wafer polishing. Moreover, atomic-precision exfoliation at the 2D interface allows for the recycling of the wafers for subsequent membrane production, with the potential for greatly reducing the manufacturing cost.

Vertical full-colour micro-LEDs via 2D materials-based layer transfer.

Micro-LEDs (µLEDs) have been explored for augmented and virtual reality display applications that require extremely high pixels per inch and luminance1,2. However, conventional manufacturing processes based on the lateral assembly of red, green and blue (RGB) µLEDs have limitations in enhancing pixel density3-6. Recent demonstrations of vertical µLED displays have attempted to address this issue by stacking freestanding RGB LED membranes and fabricating top-down7-14, but minimization of the lateral dimensions of stacked µLEDs has been difficult. Here we report full-colour, vertically stacked µLEDs that achieve, to our knowledge, the highest array density (5,100 pixels per inch) and the smallest size (4 µm) reported to date. This is enabled by a two-dimensional materials-based layer transfer technique15-18 that allows the growth of RGB LEDs of near-submicron thickness on two-dimensional material-coated substrates via remote or van der Waals epitaxy, mechanical release and stacking of LEDs, followed by top-down fabrication. The smallest-ever stack height of around 9 µm is the key enabler for record high µLED array density. We also demonstrate vertical integration of blue µLEDs with silicon membrane transistors for active matrix operation. These results establish routes to creating full-colour µLED displays for augmented and virtual reality, while also offering a generalizable platform for broader classes of three-dimensional integrated devices.

Non-epitaxial single-crystal 2D material growth by geometric confinement.

Two-dimensional (2D) materials and their heterostructures show a promising path for next-generation electronics1-3. Nevertheless, 2D-based electronics have not been commercialized, owing mainly to three critical challenges: i) precise kinetic control of layer-by-layer 2D material growth, ii) maintaining a single domain during the growth, and iii) wafer-scale controllability of layer numbers and crystallinity. Here we introduce a deterministic, confined-growth technique that can tackle these three issues simultaneously, thus obtaining wafer-scale single-domain 2D monolayer arrays and their heterostructures on arbitrary substrates. We geometrically confine the growth of the first set of nuclei by defining a selective growth area via patterning SiO2 masks on two-inch substrates. Owing to substantial reduction of the growth duration at the micrometre-scale SiO2 trenches, we obtain wafer-scale single-domain monolayer WSe2 arrays on the arbitrary substrates by filling the trenches via short growth of the first set of nuclei, before the second set of nuclei is introduced, thus without requiring epitaxial seeding. Further growth of transition metal dichalcogenides with the same principle yields the formation of single-domain MoS2/WSe2 heterostructures. Our achievement will lay a strong foundation for 2D materials to fit into industrial settings.

Suppressing ion migration in metal halide perovskite via interstitial doping with a trace amount of multivalent cations.

Cations with suitable sizes to occupy an interstitial site of perovskite crystals have been widely used to inhibit ion migration and promote the performance and stability of perovskite optoelectronics. However, such interstitial doping inevitably leads to lattice microstrain that impairs the long-range ordering and stability of the crystals, causing a sacrificial trade-off. Here, we unravel the evident influence of the valence states of the interstitial cations on their efficacy to suppress the ion migration. Incorporation of a trivalent neodymium cation (Nd3+) effectively mitigates the ion migration in the perovskite lattice with a reduced dosage (0.08%) compared to a widely used monovalent cation dopant (Na+, 0.45%). The photovoltaic performances and operational stability of the prototypical perovskite solar cells are enhanced with a trace amount of Nd3+ doping while minimizing the sacrificial trade-off.

Graphene nanopattern as a universal epitaxy platform for single-crystal membrane production and defect reduction.

Heterogeneous integration of single-crystal materials offers great opportunities for advanced device platforms and functional systems1. Although substantial efforts have been made to co-integrate active device layers by heteroepitaxy, the mismatch in lattice polarity and lattice constants has been limiting the quality of the grown materials2. Layer transfer methods as an alternative approach, on the other hand, suffer from the limited availability of transferrable materials and transfer-process-related obstacles3. Here, we introduce graphene nanopatterns as an advanced heterointegration platform that allows the creation of a broad spectrum of freestanding single-crystalline membranes with substantially reduced defects, ranging from non-polar materials to polar materials and from low-bandgap to high-bandgap semiconductors. Additionally, we unveil unique mechanisms to substantially reduce crystallographic defects such as misfit dislocations, threading dislocations and antiphase boundaries in lattice- and polarity-mismatched heteroepitaxial systems, owing to the flexibility and chemical inertness of graphene nanopatterns. More importantly, we develop a comprehensive mechanics theory to precisely guide cracks through the graphene layer, and demonstrate the successful exfoliation of any epitaxial overlayers grown on the graphene nanopatterns. Thus, this approach has the potential to revolutionize the heterogeneous integration of dissimilar materials by widening the choice of materials and offering flexibility in designing heterointegrated systems.

Self-powered image array composed of touch-free sensors fabricated with semiconductor nanowires.

We successfully develop a self-powered image array (IA) composed of 16 touch-free sensors (TFSs) fabricated with semiconductor InN nanowires (NWs) as a response medium. Without using a power supply, the InN-NW TFS can detect the position of a human hand 30 cm away from the device surface. It also distinguishes different materials such as polyimide, Al foil, printing paper, latex, and polyvinyl chloride in non-contact mode at a distance of 1 cm. The self-powered TFS-IA clearly distinguishes square-shaped transparent polydimethylsiloxane film attached to the back of a human hand positioned 5 cm from the device, indicating the possibility for detecting changes in the surface texture of human skin, such as skin burns or skin cancer. The performance of the self-powered TFS and TFS-IA is attributed to high electrostatic induction of InN NWs by external triboelectricity resulting from the simple movement of the target object, which differs markedly from conventional sensors designed to detect variations in the temperature or light essentially using a power supply.

Chip-less wireless electronic skins by remote epitaxial freestanding compound semiconductors.

Recent advances in flexible and stretchable electronics have led to a surge of electronic skin (e-skin)-based health monitoring platforms. Conventional wireless e-skins rely on rigid integrated circuit chips that compromise the overall flexibility and consume considerable power. Chip-less wireless e-skins based on inductor-capacitor resonators are limited to mechanical sensors with low sensitivities. We report a chip-less wireless e-skin based on surface acoustic wave sensors made of freestanding ultrathin single-crystalline piezoelectric gallium nitride membranes. Surface acoustic wave-based e-skin offers highly sensitive, low-power, and long-term sensing of strain, ultraviolet light, and ion concentrations in sweat. We demonstrate weeklong monitoring of pulse. These results present routes to inexpensive and versatile low-power, high-sensitivity platforms for wireless health monitoring devices.

Long-term reliable physical health monitoring by sweat pore-inspired perforated electronic skins.

Electronic skins (e-skins)-electronic sensors mechanically compliant to human skin-have long been developed as an ideal electronic platform for noninvasive human health monitoring. For reliable physical health monitoring, the interface between the e-skin and human skin must be conformal and intact consistently. However, conventional e-skins cannot perfectly permeate sweat in normal day-to-day activities, resulting in degradation of the intimate interface over time and impeding stable physical sensing. Here, we present a sweat pore-inspired perforated e-skin that can effectively suppress sweat accumulation and allow inorganic sensors to obtain physical health information without malfunctioning. The auxetic dumbbell through-hole patterns in perforated e-skins lead to synergistic effects on physical properties including mechanical reliability, conformability, areal mass density, and adhesion to the skin. The perforated e-skin allows one to laminate onto the skin with consistent homeostasis, enabling multiple inorganic sensors on the skin to reliably monitor the wearer's health over a period of weeks.

Impact of 2D-3D Heterointerface on Remote Epitaxial Interaction through Graphene.

Remote epitaxy has drawn attention as it offers epitaxy of functional materials that can be released from the substrates with atomic precision, thus enabling production and heterointegration of flexible, transferrable, and stackable freestanding single-crystalline membranes. In addition, the remote interaction of atoms and adatoms through two-dimensional (2D) materials in remote epitaxy allows investigation and utilization of electrical/chemical/physical coupling of bulk (3D) materials via 2D materials (3D-2D-3D coupling). Here, we unveil the respective roles and impacts of the substrate material, graphene, substrate-graphene interface, and epitaxial material for electrostatic coupling of these materials, which governs cohesive ordering and can lead to single-crystal epitaxy in the overlying film. We show that simply coating a graphene layer on wafers does not guarantee successful implementation of remote epitaxy, since atomically precise control of the graphene-coated interface is required, and provides key considerations for maximizing the remote electrostatic interaction between the substrate and adatoms. This was enabled by exploring various material systems and processing conditions, and we demonstrate that the rules of remote epitaxy vary significantly depending on the ionicity of material systems as well as the graphene-substrate interface and the epitaxy environment. The general rule of thumb discovered here enables expanding 3D material libraries that can be stacked in freestanding form.

Activation of ß-catenin by TGF-ß1 promotes ligament-fibroblastic differentiation and inhibits cementoblastic differentiation of human periodontal ligament cells.

TGF-ß and Wnt/ß-catenin signaling pathways are known to be essential for the development of periodontal tissue. In this study, we examined the crosstalk between TGF-ß and Wnt/ß-catenin signaling in ligament-fibroblastic differentiation of human periodontal ligament cells (hPDLCs). TGF-ß1 treatment significantly increased the expression of ligament-fibroblastic markers, but such expression was preventing by treatment with SB431542, a TGF-ß type I receptor inhibitor. As well as phosphorylation of Smad3, TGF-ß1 increased ß-catenin activation. The depletion of ß-catenin reduced the expression of ligament-fibroblastic markers, suggesting that ß-catenin is essential for ligament differentiation. The effect of TGF-ß1 on ß-catenin activation did not seem to be much correlated with Wnt stimuli, but endogenous DKK1 was suppressed by TGF-ß1, indicating that ß-catenin activation could be increased much more by TGF-ß1. In addition to DKK1 suppression, Smad3 phosphorylation by TGF-ß1 facilitated the nuclear translocation of cytoplasmic ß-catenin. In contrast to ligament-fibroblastic differentiation, inhibition of TGF-ß1 signaling was needed for cementoblastic differentiation of hPDLCs. BMP7 treatment accompanied by inhibition of TGF-ß1 signaling had a synergistic effect on cementoblastic differentiation. In conclusion, ß-catenin activation by TGF-ß1 caused ligament-fibroblastic differentiation of hPDLCs, and the presence of TGF-ß1 stimuli basically determined whether hPDLCs are differentiated into ligament progenitor or cementoblasts.

Ledge-directed epitaxy of continuously self-aligned single-crystalline nanoribbons of transition metal dichalcogenides.

Two-dimensional transition metal dichalcogenide nanoribbons are touted as the future extreme device downscaling for advanced logic and memory devices but remain a formidable synthetic challenge. Here, we demonstrate a ledge-directed epitaxy (LDE) of dense arrays of continuous, self-aligned, monolayer and single-crystalline MoS2 nanoribbons on ß-gallium (III) oxide (ß-Ga2O3) (100) substrates. LDE MoS2 nanoribbons have spatial uniformity over a long range and transport characteristics on par with those seen in exfoliated benchmarks. Prototype MoS2-nanoribbon-based field-effect transistors exhibit high on/off ratios of 108 and an averaged room temperature electron mobility of 65 cm2 V-1 s-1. The MoS2 nanoribbons can be readily transferred to arbitrary substrates while the underlying ß-Ga2O3 can be reused after mechanical exfoliation. We further demonstrate LDE as a versatile epitaxy platform for the growth of p-type WSe2 nanoribbons and lateral heterostructures made of p-WSe2 and n-MoS2 nanoribbons for futuristic electronics applications.

Hybrid Integrated Photomedical Devices for Wearable Vital Sign Tracking.

In light of the importance of and challenges inherent in realizing a wearable healthcare platform for simultaneously recognizing, preventing, and treating diseases while tracking vital signs, the development of simple and customized functional devices has been required. Here, we suggest a new approach for making a stretchable light waveguide which can be combined with integrated functional devices, such as organic photodetectors (PDs) and nanowire-based heaters, for multifunctional healthcare monitoring. Controlling the reflection condition of the medium gave a solid design rule for strong light emission in our stretchable waveguides. Based on this rule, the stretchable light waveguide (up to 50% strain) made of polydimethylsiloxane was successfully demonstrated with strong emissions. We also incorporated highly sensitive organic PDs and silver nanowire-based heaters with the stretchable waveguide for the detection of vital signs, including the heart rate, deep breathing, coughs, and blood oxygen saturation. Through these multifunctional performances, we have successfully demonstrated that our stretchable light waveguide has a strong potential for multifunctional healthcare monitoring.

Heterogeneous integration of single-crystalline complex-oxide membranes.

Complex-oxide materials exhibit a vast range of functional properties desirable for next-generation electronic, spintronic, magnetoelectric, neuromorphic, and energy conversion storage devices1-4. Their physical functionalities can be coupled by stacking layers of such materials to create heterostructures and can be further boosted by applying strain5-7. The predominant method for heterogeneous integration and application of strain has been through heteroepitaxy, which drastically limits the possible material combinations and the ability to integrate complex oxides with mature semiconductor technologies. Moreover, key physical properties of complex-oxide thin films, such as piezoelectricity and magnetostriction, are severely reduced by the substrate clamping effect. Here we demonstrate a universal mechanical exfoliation method of producing freestanding single-crystalline membranes made from a wide range of complex-oxide materials including perovskite, spinel and garnet crystal structures with varying crystallographic orientations. In addition, we create artificial heterostructures and hybridize their physical properties by directly stacking such freestanding membranes with different crystal structures and orientations, which is not possible using conventional methods. Our results establish a platform for stacking and coupling three-dimensional structures, akin to two-dimensional material-based heterostructures, for enhancing device functionalities8,9.

Graphene-assisted spontaneous relaxation towards dislocation-free heteroepitaxy.

Although conventional homoepitaxy forms high-quality epitaxial layers1-5, the limited set of material systems for commercially available wafers restricts the range of materials that can be grown homoepitaxially. At the same time, conventional heteroepitaxy of lattice-mismatched systems produces dislocations above a critical strain energy to release the accumulated strain energy as the film thickness increases. The formation of dislocations, which severely degrade electronic/photonic device performances6-8, is fundamentally unavoidable in highly lattice-mismatched epitaxy9-11. Here, we introduce a unique mechanism of relaxing misfit strain in heteroepitaxial films that can enable effective lattice engineering. We have observed that heteroepitaxy on graphene-coated substrates allows for spontaneous relaxation of misfit strain owing to the slippery graphene surface while achieving single-crystalline films by reading the atomic potential from the substrate. This spontaneous relaxation technique could transform the monolithic integration of largely lattice-mismatched systems by covering a wide range of the misfit spectrum to enhance and broaden the functionality of semiconductor devices for advanced electronics and photonics.