Metastable states of 2D-material-on-metal-islands structures revealed by thermal cycling

TL;DR

This study investigates the thermal stability of van der Waals bonds in 2D material heterostructures on metal islands, revealing irreversible changes upon thermal cycling and methods for restoring contact, with implications for device reliability.

Contribution

It provides new insights into the metastability and interfacial stability of 2D heterostructures under thermal cycling, highlighting the role of thermal expansion and residues.

Findings

Thermal cycling causes irreversible degradation of metal-graphene contact.

Hot pressing can restore the metal-graphene interface.

Interfacial water or residues influence metastability.

Abstract

The integration of 2D materials with artificially textured substrates offers exceptional opportunities for engineering novel functional devices. A straightforward technological route towards such devices is a mechanical dry or wet transfer of 2D layer or heterostructure onto prepared patterned elements with subsequent van der Waals bonding. An issue of van der Waals bond stability is crucial for device operation but is almost unexplored. In our research we address it by studying transport properties of hBN/graphene heterostructures transferred onto metallic island arrays and subjected to thermal cycling. We reveal that heating from cryogenic to room temperature and cooling back leads to irreversible changes in electronic transport properties: the contact between metal and graphene degrades, and signatures of suspended graphene regions transport disappear. These changes are accompanied by slight movement of the flakes and atomic-force-microscope-detected breakdown of van der Waals bonds between the flake and substrate near the metal electrodes. Interestingly, a hot pressing allows to restore the metal-to-graphene contact. We relate the observed metastability to the thermal-expansion-driven flake delamination and argue that it is accompanied by redistribution of the interfacial water or organic residues. Our findings provide useful insights into the topic of interfacial stability in van der Waals heterostructures and establish constraints for low-temperature applications of transferred 2D devices. We also add up an additional control parameter for the experimentalists in the field of 2D materials - degree of quenched disorder.