All-dry flip-over stacking of van der Waals junctions of 2D materials using polyvinyl chloride.

We demonstrated an all-dry polymer-to-polymer transfer technique for two-dimensional (2D) crystal flakes using a polyvinyl chloride (PVC) layer deposited on a piece of polydimethylsiloxane (PDMS). Unexpectedly, the pickup/release temperatures were modified in wider temperature range simply by changing the thickness of the PVC layer than changing the plasticizer ratio. Utilizing the difference in the pickup/release temperatures depending on the PVC film thickness, 2D flakes were transferred from a thicker PVC film to a thinner one. This polymer-to-polymer transfer technique can be utilized to flip over van der Waals heterostructures. As a demonstration, we fabricated a mountain-like stacked structure of hexagonal boron nitride flakes using the flip-over stacking technique. Finally, we compared the results of thermomechanical analysis with the pickup/release temperatures of the PVC/PDMS stamp. The PVC was revealed to be at the glass transition and in the viscoelastic flow regimes when the 2D flakes were picked up and dry released, respectively. Our polymer-to-polymer transfer method facilitates flip-over van der Waals stacking in an all-dry manner, expanding the possibility of 2D materials device fabrications.

Dry pick-and-flip assembly of van der Waals heterostructures for microfocus angle-resolved photoemission spectroscopy.

We present a dry pick-and-flip assembly technique for angle-resolved photoemission spectroscopy (ARPES) of van der Waals heterostructures. By combining Elvacite2552C acrylic resin and 1-ethyl-3-methylimidazolium ionic liquid, we prepared polymers with glass transition temperatures (Tg) ranging from 37 to 100 â„ƒ. The adhesion of the polymer to the 2D crystals was enhanced at [Formula: see text]. By utilizing the difference in [Formula: see text], a 2D heterostructure can be transferred from a high-[Formula: see text] polymer to a lower-[Formula: see text] polymer, which enables flipping its surface upside down. This process is suitable for assembling heterostructures for ARPES, where the top capping layer should be monolayer graphene. The laser-based micro-focused ARPES measurements of 5-layer WTe2, 3-layer MoTe2, 2-layer WTe2/few-layer Cr2Ge2Te6, and twisted double bilayer WTe2 demonstrate that this process can be utilized as a versatile sample fabrication method for investigating the energy spectra of 2D heterostructures.

3D Manipulation of 2D Materials Using Microdome Polymer.

We demonstrate 3D mechanical manipulations, such as sliding, rotating, folding, flipping, and exfoliating, of 2D materials using a microdome polymer (MDP) via in situ real-time observation with an optical microscope. A dimethylpolysiloxane (PDMS)-based MDP is covered with a poly(vinyl chloride) (PVC) adhesion layer. This PVC-MDP structure enables us to achieve small and adjustable contact areas between the PVC-MDP and a 2D-material flake, which is typically between ∼10 and ∼100 µm in diameter. The adhesion between the PVC polymer and 2D materials is fully tunable with temperature: Strong adhesion at ∼70 °C allows pick-up of the 2D material, and release occurs at ∼130 °C when the adhesion is weak. Thus the PVC-MDP functions as a point-of-contact manipulator for 2D materials, permitting the 3D manipulation of 2D-material flakes. Our method could facilitate the expansion of van der Waals heterostructure fabrication technology and the development of preparation techniques for more complex 3D structures.