Band offsets and stability of WSe$_2$/RuCl$_3$ van der Waals charge-transfer contacts

Abstract

The layered Mott insulator $α$-RuCl$_3$ induces degenerate hole-doping in two-dimensional semiconductors due to its large electron affinity, making it a promising charge-transfer material for establishing ohmic contacts in electronic devices. In order to assess the applicability and guide the design of devices incorporating RuCl$_3$ it is critical to determine the electronic structure and robustness of the band offsets that underpin the transport properties of semiconductors in contact with RuCl$_3$. Here, we apply micro-focused angle-resolved photoemission spectroscopy to determine the electronic structure of single-layer WSe$_2$ contacted to RuCl$_3$ on hexagonal boron nitride substrates. We find that formation of a functioning WSe$_2$/RuCl$_3$ contact leads to a valence band shift of $(0.68 \pm 0.05)$ eV towards the Fermi energy in WSe$_2$. The charge transfer effect is challenging to observe as it depends sensitively on fabrication conditions such as solvent exposure, quality of interface encapsulation and heating of RuCl$_3$, imposing strict requirements on device design to attain high-quality contacts.