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Biomorph actuators composed of two layers with asymmetric thermal expansion properties are widely explored owing to their high mechanical adaptability. Electrothermal nanomaterials are employed as the Joule heating components in them for controlled thermal expansion, while their large integration thickness often limits resulting actuation performances. This study reports high‐performance ultrathin soft biomorph actuators enabled by near atom‐thickness 2D platinum ditelluride (PtTe₂) layers—a new class of emergent metallic 2D transition metal dichalcogenides. The actuators employ wafer‐scale 2D PtTe₂layers sandwiched in between two polymer films of largely mismatched thermal expansion coefficients, which are electrically biased to generate Joule heating. This electrical‐to‐thermal conversion causes the asymmetric expansion of the polymers achieving outstanding actuation motions; i.e., large bending curvature, fast responsiveness, as well as high reversibility and endurance, which surpass the performances of previously explored graphene‐based actuators with much smaller dimensions. Furthermore, the 2D PtTe₂layers‐enabled actuators are demonstrated to function as soft grippers in lifting and relocating heavier objects, implying the great potential of near atom‐thickness materials in biomimetic devices.

 

Heterogeneous integrations of functionally and chemically distinct materials have been explored to develop promising building blocks for opto‐electronic device applications. Recently, the Van der Waals (vdW)‐assembly of near atom thickness materials has provided excellent opportunities beyond what has been previously been difficult to realize. However, its up‐to‐date demonstrations remain far from achieving the scalability and versatility demanded for practical device applications, that is, the integration is generally demonstrated with intrinsically layered 2D materials of very small lateral dimensions. Herein, the large centimeter‐scale vdW assembly of two different materials with structurally, chemically, and functionally distinct properties, that is, 2D platinum ditelluride (PtTe₂) metallic multilayers and non‐layered 3D semiconducting platinum sulfide (PtS) are reported. Both materials are precisely delaminated from their growth wafers inside water and are subsequently integrated on unconventional substrates of desired functionalities. The large‐area vdW‐assembled 2D/3D PtTe₂/PtS hetero‐materials on flexible substrates exhibit an excellent photodetection in a spectral range of visible‐to‐near infrared (NIR) wavelength, which is well preserved under severe mechanical deformation. This study paves the way for exploring large‐area flexible opto‐electronic devices solely based on near atom thickness materials.

 

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.

 

Two-dimensional (2D) molybdenum disulfide (MoS 2 ) layers are suitable for visible-to-near infrared photodetection owing to their tunable optical bandgaps. Also, their superior mechanical deformability enabled by an extremely small thickness and van der Waals (vdW) assembly allows them to be structured into unconventional physical forms, unattainable with any other materials. Herein, we demonstrate a new type of 2D MoS 2 layer-based rollable photodetector that can be mechanically reconfigured while maintaining excellent geometry-invariant photo-responsiveness. Large-area (>a few cm 2 ) 2D MoS 2 layers grown by chemical vapor deposition (CVD) were integrated on transparent and flexible substrates composed of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNs) by a direct solution casting method. These composite materials in three-dimensionally rollable forms exhibited a large set of intriguing photo-responsiveness, well preserving intrinsic opto-electrical characteristics of the integrated 2D MoS 2 layers; i.e. , light intensity-dependent photocurrents insensitive to illumination angles as well as highly tunable photocurrents varying with the rolling number of 2D MoS 2 layers, which were impossible to achieve with conventional photodetectors. This study provides a new design principle for converting 2D materials to three-dimensional (3D) objects of tailored functionalities and structures, significantly broadening their potential and versatility in futuristic devices. 

2D PtTe 2 layers, a relatively new class of 2D crystals, have unique band structure and remarkably high electrical conductivity promising for emergent opto-electronics. This intrinsic superiority can be further leveraged toward practical device applications by merging them with mature 3D semiconductors, which has remained largely unexplored. Herein, we explored 2D/3D heterojunction devices by directly growing large-area (>cm 2 ) 2D PtTe 2 layers on Si wafers using a low-temperature CVD method and unveiled their superior opto-electrical characteristics. The devices exhibited excellent Schottky transport characteristics essential for high-performance photovoltaics and photodetection, i.e. , well-balanced combination of high photodetectivity (>10 13 Jones), small photo-responsiveness time (∼1 μs), high current rectification ratio (>10 5 ), and water super-hydrophobicity driven photovoltaic improvement (>300%). These performances were identified to be superior to those of previously explored 2D/3D or 2D layer-based devices with much smaller junction areas, and their underlying principles were confirmed by DFT calculations.