The key to achieve high-quality van der Waals heterostructure devices made of stacking various two-dimensional (2D) layered materials lies in the clean interface without bubbles and wrinkles. Although polymethylmethacrylate (PMMA) is generally used as a sacrificial transfer film due to its strong adhesion property, it is always dissolved in the solvent after the transfer, resulting in the unavoidable PMMA residue on the top surface. This makes it difficult to locate clean interface areas. In this work, we present a fully dry PMMA transfer of graphene onto h-BN using a heating/cooling system which allows identification of clean interface area for high quality graphene/h-BN heterostructure fabrication. The mechanism lies in the utilization of the large difference in thermal expansion coefficients between polymers (PMMA/PDMS) and inorganic materials (graphene/h-BN substrate) to mechanically peel off PMMA from graphene by the thermal shrinkage of polymers, leaving no PMMA residue on the graphene surface. This method can be applied to all types of 2D layered materials.

The key to achieving high-quality van der Waals heterostructure devices made by stacking twodimensional (2D) layered materials lies in having a clean interface without interfacial bubbles and wrinkles. In this study, the pinpoint pick-up and transfer system of 2D crystals is constructed using polymers with lens shapes. We report the bubble-free and clean-interface assembly of 2D crystals in which unidirectional sweep of the transfer interface precisely controlled with the help of the inclined substrate pushes the bubbles away from the interface.

Bilayer graphene field effect transistors (BLG-FETs), unlike conventional semiconductors, are greatly sensitive to potential fluctuations because of the charged impurities in high- k gate stacks because the potential difference between two layers induced by the external perpendicular electrical filed is the physical origin behind the band gap opening. The assembly of BLG with layered h-BN insulators into a van der Waals heterostructure has been widely recognized to achieve the superior electrical transport properties. However, the carrier response properties at the h-BN/BLG heterointerface, which control the device performance, have not yet been revealed because of the inevitably large parasitic capacitance. In this study, the significant reduction of potential fluctuations to ∼1 meV is achieved in an all-two-dimensional heterostructure BLG-FET on a quartz substrate, which results in the suppression of the off-current to the measurement limit at a small band gap of ∼90 meV at 20 K. By capacitance measurement, we demonstrate that the electron trap/detrap response at such heterointerface is suppressed to undetectable level in the measurement frequency range. The electrically inert van der Waals heterointerface paves the way for the realization of future BLG electronics applications.

Controlling the stacking order in bilayer graphene (BLG) allows realizing interesting physical properties. In particular, the possibility of tuning the band gap in Bernal-stacked (AB) BLG (AB-BLG) has a great technological importance for electronic and optoelectronic applications. Most of the current methods to produce AB-BLG suffer from inhomogeneous layer thickness and/or coexistence with twisted BLG. Here, we demonstrate a method to synthesize highly pure large-area AB-BLG by chemical vapor deposition using Cu–Ni films. Increasing the reaction time resulted in a gradual increase of the AB stacking, with the BLG eventually free from twist regions for the longer growth times (99.4% of BLG has AB stacking), due to catalyst-assisted continuous BLG reconstruction driven by carbon dissolution–segregation processes. The band gap opening was confirmed by the electrical measurements on field-effect transistors using two different device configurations. The concept of the continuous reconstruction to achieve highly pure AB-BLG offers a way to control the stacking order of catalytically grown two-dimensional materials.

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