Polymer-Free Assembly of Unencapsulated van der Waals Heterostructure Devices

Abstract van der Waals (vdW) heterostructures provide a versatile platform for exploring emergent quantum phenomena, yet their fabrication is often limited by interfacial contamination and incompatibility with surface-sensitive characterization. Here, we demonstrate muscovite mica as a polymer-free platform for assembling and patterning vdW heterostructure devices. Mica-mediated transfer enables clean exposed surfaces suitable for atomic-resolution scanning tunneling microscopy (STM) following mild thermal annealing, without aggressive postprocessing. Mica also serves as a mechanically robust support for sequential pickup assembly, eliminating intermediate release steps. Furthermore, exfoliated mica flakes function as removable shadow masks for contact deposition, enabling straightforward patterning without conventional lithography. We quantify the temperature dependence of mica-mediated graphene pickup and demonstrate gate-dependent transport in a three-terminal graphene/hBN device fabricated using the approach. By integrating transfer, sequential assembly, and contact patterning within a single materials platform, mica provides a simple and accessible route to unencapsulated vdW heterostructures for surface-sensitive spectroscopy and quantum-device applications.