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The interplay between the strong intralayer covalent-ionic bonds and the weak interlayer van der Waals (vdW) forces between the neighboring layers of vdW crystals gives rise to unique physical and chemical properties. Here, the intralayer and interlayer bondings in ? and ? polytypes of In2Se3 are studied, a vdW material with potential applications in advanced electronic and optical devices. Picosecond ultrasonic experiments are conducted to probe the sound velocity in the direction perpendicular to the vdW layers. The measured sound velocities are different in ?- and ?-In2Se3, suggesting a significant difference in their elastic properties. Density functional theory and an effective spring model are used to calculate the elastic stiffness of the layer and vdW gap in ?- and ?-In2Se3. The calculated elastic moduli show good agreement with experimental values and reveal the dominant contribution of interlayer atomic bonding to the different elastic properties of the two polytypes. The findings show the power of picosecond ultrasonics for probing the fundamental elastic properties of vdW materials. The data and analysis also provide a reliable description of the intra- and interlayer forces in complex crystal structures, such as the polytype phases of In2Se3.

© 2020 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH 2D materials have unique structural and electronic properties with potential for transformative device applications. However, such devices are usually bespoke structures made by sequential deposition of exfoliated 2D layers. There is a need for scalable manufacturing techniques capable of producing high-quality large-area devices comprising multiple 2D materials. Additive manufacturing with inks containing 2D material flakes is a promising solution. Inkjet-printed devices incorporating 2D materials have been demonstrated, however there is a need for greater understanding of quantum transport phenomena as well as their structural properties. Experimental and theoretical studies of inkjet-printed graphene structures are presented. Detailed electrical and structural characterization is reported and explained by comparison with transport modeling that include inter-flake quantum tunneling transport and percolation dynamics. The results reveal that the electrical properties are strongly influenced by the flakes packing fraction and by complex meandering electron trajectories, which traverse several printed layers. Controlling these trajectories is essential for printing high-quality devices that exploit the properties of 2D materials. Inkjet-printed graphene is used to make a field effect transistor and Ohmic contacts on an InSe phototransistor. This is the first time that inkjet-printed graphene has successfully replaced single layer graphene as a contact material for 2D metal chalcogenides.