Two-dimensional (2D) transition-metal dichalcogenides (2D TMDs) in the form of MX2 (M: transition metal, X: chalcogen) exhibit intrinsically anisotropic layered crystallinity wherein their material properties are determined by constituting M and X elements. 2D platinum diselenide (2D PtSe2) is a relatively unexplored class of 2D TMDs with noble-metal Pt as M, offering distinct advantages over conventional 2D TMDs such as higher carrier mobility and lower growth temperatures. Despite the projected promise, much of its fundamental structural and electrical properties and their interrelation have not been clarified, and so its full technological potential remains mostly unexplored. In this work, we investigate the structural evolution of large-area chemical vapor deposition (CVD)-grown 2D PtSe2 layers of tailored morphology and clarify its influence on resulting electrical properties. Specifically, we unveil the coupled transition of structural–electrical properties in 2D PtSe2 layers grown at a low temperature (i.e., 400 °C). The layer orientation of 2D PtSe2 grown by the CVD selenization of seed Pt films exhibits horizontal-to-vertical transition with increasing Pt thickness. While vertically aligned 2D PtSe2 layers present metallic transports, field-effect-transistor gate responses were observed with thin horizontally aligned 2D PtSe2 layers prepared with Pt of small thickness. Density functional theory calculation identifies the electronic structures of 2D PtSe2 layers undergoing the transition of horizontal-to-vertical layer orientation, further confirming the presence of this uniquely coupled structural-electrical transition. The advantage of low-temperature growth was further demonstrated by directly growing 2D PtSe2 layers of controlled orientation on polyimide polymeric substrates and fabricating their Kirigami structures, further strengthening the application potential of this material. Discussions on the growth mechanism behind the horizontal-to-vertical 2D layer transition are also presented.

Non‐volatile resistive switching (NVRS) is a widely available effect in transitional metal oxides, colloquially known as memristors, and of broad interest for memory technology and neuromorphic computing. Until recently, NVRS was not known in other transitional metal dichalcogenides (TMDs), an important material class owing to their atomic thinness enabling the ultimate dimensional scaling. Here, various monolayer or few‐layer 2D materials are presented in the conventional vertical structure that exhibit NVRS, including TMDs (MX2, M = transitional metal, e.g., Mo, W, Re, Sn, or Pt; X = chalcogen, e.g., S, Se, or Te), TMD heterostructure (WS2/MoS2), and an atomically thin insulator (h‐BN). These results indicate the universality of the phenomenon in 2D non‐conductive materials, and feature low switching voltage, large ON/OFF ratio, and forming‐free characteristic. A dissociation–diffusion–adsorption model is proposed, attributing the enhanced conductance to metal atoms/ions adsorption into intrinsic vacancies, a conductive‐point mechanism supported by first‐principle calculations and scanning tunneling microscopy characterizations. The results motivate further research in the understanding and applications of defects in 2D materials.

Platinum ditelluride (PtTe2) is an emerging semimetallic two-dimensional (2D) transition-metal dichalcogenide (TMDC) crystal with intriguing band structures and unusual topological properties. Despite much devoted efforts, scalable and controllable synthesis of large-area 2D PtTe2 with well-defined layer orientation has not been established, leaving its projected structure–property relationship largely unclarified. Herein, we report a scalable low-temperature growth of 2D PtTe2 layers on an area greater than a few square centimeters by reacting Pt thin films of controlled thickness with vaporized tellurium at 400 °C. We systematically investigated their thickness-dependent 2D layer orientation as well as its correlated electrical conductivity and surface property. We unveil that 2D PtTe2 layers undergo three distinct growth mode transitions, i.e., horizontally aligned holey layers, continuous layer-by-layer lateral growth, and horizontal-to-vertical layer transition. This growth transition is a consequence of competing thermodynamic and kinetic factors dictated by accumulating internal strain, analogous to the transition of Frank–van der Merwe (FM) to Stranski–Krastanov (SK) growth in epitaxial thin-film models. The exclusive role of the strain on dictating 2D layer orientation has been quantitatively verified by the transmission electron microscopy (TEM) strain mapping analysis. These centimeter-scale 2D PtTe2 layers exhibit layer orientation tunable metallic transports yielding the highest value of ∼1.7 × 106 S/m at a certain critical thickness, supported by a combined verification of density functional theory (DFT) and electrical measurements. Moreover, they show intrinsically high hydrophobicity manifested by the water contact angle (WCA) value up to ∼117°, which is the highest among all reported 2D TMDCs of comparable dimensions and geometries. Accordingly, this study confirms the high material quality of these emerging large-area 2D PtTe2 layers, projecting vast opportunities employing their tunable layer morphology and semimetallic properties from investigations of novel quantum phenomena to applications in electrocatalysis.

Wearable bioelectronics with emphasis on the research and development of advanced person-oriented biomedical devices have attracted immense interest in the last decade.Scientists and clinicians find it essential to utilize skin-worn smart tattoos for on-demand and ambulatory monitoring of an individual's vital signs. Here we report on the development of novel ultrathin platinum-based two-dimensional dichalcogenide (Pt-TMDs) based electronic tattoos as advanced building blocks of future wearable bioelectronics. We made these ultrathin electronic tattoos out of large-scale synthesized platinum diselenide (PtSe2) and platinum ditelluride (PtTe2) layered materials and used them for monitoring human physiological vital signs, such as the electrical activity of the heart and the brain, muscle contractions, eye movements, and temperature.We show that both materials can be used for these applications; yet, PtTe2 was found to be the most suitable choice due to its metallic structure. In terms of sheet resistance, skin-contact, and electrochemical impedance, PtTe2 outperforms state-of-the-art gold and graphene electronic tattoos and performs on par with medical-grade Ag/AgCl gel electrodes. The PtTe2 tattoos show four times lower impedance and almost 100 times lower sheet resistance compared to monolayer graphene tattoos. One of the possible prompt implications of the work is perhaps in the development of advanced human-machine interfaces. To display the application, we built a multitattoo system that can easily distinguish eye movement and identify the direction of an individual's sight.

Two-dimensional transition-metal dichalcogenide (2D TMD) layers are highly attractive for emerging stretchable and foldable electronics owing to their extremely small thickness coupled with extraordinary electrical and optical properties. Although intrinsically large strain limits are projected in them (i.e., several times greater than silicon), integrating 2D TMDs in their pristine forms does not realize superior mechanical tolerance greatly demanded in high-end stretchable and foldable devices of unconventional form factors. In this article, we report a versatile and rational strategy to convert 2D TMDs of limited mechanical tolerance to tailored 3D structures with extremely large mechanical stretchability accompanying well-preserved electrical integrity and modulated transport properties. We employed a concept of strain engineering inspired by an ancient paper-cutting art, known as kirigami patterning, and developed 2D TMD-based kirigami electrical conductors. Specifically, we directly integrated 2D platinum diselenide (2D PtSe2) layers of controlled carrier transport characteristics on mechanically flexible polyimide (PI) substrates by taking advantage of their low synthesis temperature. The metallic 2D PtSe2/PI kirigami patterns of optimized dimensions exhibit an extremely large stretchability of ∼2000% without compromising their intrinsic electrical conductance. They also present strain-tunable and reversible photoresponsiveness when interfaced with semiconducting carbon nanotubes (CNTs), benefiting from the formation of 2D PtSe2/CNT Schottky junctions. Moreover, kirigami field-effect transistors (FETs) employing semiconducting 2D PtSe2 layers exhibit tunable gate responses coupled with mechanical stretching upon electrolyte gating. The exclusive role of the kirigami pattern parameters in the resulting mechanoelectrical responses was also verified by a finite-element modeling (FEM) simulation. These multifunctional 2D materials in unconventional yet tailored 3D forms are believed to offer vast opportunities for emerging electronics and optoelectronics.

Two-dimensional (2D) transition metal dichalcogenide (2D TMD) layers present an unusually ideal combination of excellent opto-electrical properties and mechanical tolerance projecting high promise for a wide range of emerging applications, particularly in flexible and stretchable devices. The prerequisite for realizing such opportunities is to reliably integrate large-area 2D TMDs of well-defined dimensions on mechanically pliable materials with targeted functionalities by transferring them from rigid growth substrates. Conventional approaches to overcome this challenge have been limited as they often suffer from the non-scalable integration of 2D TMDs whose structural and chemical integrity are altered through toxic chemicals-involved processes. Herein, we report a generic and reliable strategy to achieve the layer-by-layer integration of large-area 2D TMDs and their heterostructure variations onto a variety of unconventional substrates. This new 2D layer integration method employs water only without involving any other chemicals, thus renders distinguishable advantages over conventional approaches in terms of material property preservation and integration size scalability. We have demonstrated the generality of this method by integrating a variety of 2D TMDs and their heterogeneously-assembled vertical layers on exotic substrates such as plastics and papers. Moreover, we have verified its technological versatility by demonstrating centimeter-scale 2D TMDs-based flexible photodetectors and pressure sensors which are difficult to fabricate with conventional approaches. Fundamental principles for the water-assisted spontaneous separation of 2D TMD layers are also discussed.

Summary Two-dimensional (2D) layered materials and their heterostructures have recently been recognized as promising building blocks for futuristic brain-like neuromorphic computing devices. They exhibit unique properties such as near-atomic thickness, dangling-bond-free surfaces, high mechanical robustness, and electrical/optical tunability. Such attributes unattainable with traditional electronic materials are particularly promising for high-performance artificial neurons and synapses, enabling energy-efficient operation, high integration density, and excellent scalability. In this review, diverse 2D materials explored for neuromorphic applications, including graphene, transition metal dichalcogenides, hexagonal boron nitride, and black phosphorous, are comprehensively overviewed. Their promise for neuromorphic applications are fully discussed in terms of material property suitability and device operation principles. Furthermore, up-to-date demonstrations of neuromorphic devices based on 2D materials or their heterostructures are presented. Lastly, the challenges associated with the successful implementation of 2D materials into large-scale devices and their material quality control will be outlined along with the future prospect of these emergent materials.

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