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.

Understanding the 2D-material and substrate interaction during epitaxial growth towards successful remote epitaxy: a review.

Remote epitaxy, which was discovered and reported in 2017, has seen a surge of interest in recent years. Although the technology seemed to be difficult to reproduce by other labs at first, remote epitaxy has come a long way and many groups are able to consistently reproduce the results with a wide range of material systems including III-V, III-N, wide band-gap semiconductors, complex-oxides, and even elementary semiconductors such as Ge. As with any nascent technology, there are critical parameters which must be carefully studied and understood to allow wide-spread adoption of the new technology. For remote epitaxy, the critical parameters are the (1) quality of two-dimensional (2D) materials, (2) transfer or growth of 2D materials on the substrate, (3) epitaxial growth method and condition. In this review, we will give an in-depth overview of the different types of 2D materials used for remote epitaxy reported thus far, and the importance of the growth and transfer method used for the 2D materials. Then, we will introduce the various growth methods for remote epitaxy and highlight the important points in growth condition for each growth method that enables successful epitaxial growth on 2D-coated single-crystalline substrates. We hope this review will give a focused overview of the 2D-material and substrate interaction at the sample preparation stage for remote epitaxy and during growth, which have not been covered in any other review to date.

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.

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.

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.

Mid-infrared photon sensing using InGaN/GaN nanodisks via intersubband absorption.

Intersubband (intraband) transitions allow absorption of photons in the infrared spectral regime, which is essential for IR-photodetector and optical communication applications. Among various technologies, nanodisks embedded in nanowires offer a unique opportunity to be utilized in intraband devices due to the ease of tuning the fundamental parameters such as strain distribution, band energy, and confinement of the active region. Here, we show the transverse electric polarized intraband absorption using InGaN/GaN nanodisks cladded by AlGaN. Fourier transform infrared reflection (FTIR) measurement confirms absorption of normal incident in-plane transverse electric polarized photons in the mid-IR regime (wavelength of ~ 15 µm) at room temperature. The momentum matrix of the nanodisk energy states indicates electron transition from the ground state s into the px or py orbital-like excited states. Furthermore, the absorption characteristics depending on the indium composition and nanowire diameter exhibits tunability of the intraband absorption spectra within the nanodisks. We believe nanodisks embedded nanowires is a promising technology for achieving tunable detection of photons in the IR spectrum.

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.

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.

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.