Laser writable high-K dielectric for van der Waals nano-electronics

This is the author accepted manuscript. The final version is available from American Association for the Advancement of Science via the DOI in this record.Like silicon-based semiconductor devices, van der Waals heterostructures will require integration with high-K oxides. This is needed to achieve suitable voltage scaling, improved performance as well as allowing for added functionalities. Unfortunately, commonly used high-k oxide deposition methods are not directly compatible with 2D materials. Here we demonstrate a method to embed a multi-functional few nm thick high-k oxide within van der Waals devices without degrading the properties of the neighbouring 2D materials. This is achieved by in-situ laser oxidation of embedded few layer HfS2 crystals. The resultant oxide is found to be in the amorphous phase with a dielectric constant of k~15 and break-down electric fields in the range of 0.5-0.6 V/nm. This transformation allows for the creation of a variety of fundamental nano-electronic and opto-electronic devices including, flexible Schottky barrier field effect transistors, dual gated graphene transistors as well as vertical light emitting and detecting tunnelling transistors. Furthermore, upon dielectric break-down, electrically conductive filaments are formed. This filamentation process can be used to electrically contact encapsulated conductive materials. Careful control of the filamentation process also allows for reversible switching between two resistance states. This allows for the creation of resistive switching random access memories (ReRAMs). We believe that this method of embedding a high-k oxide within complex van der Waals heterostructures could play an important role in future flexible multi-functional van der Waals devices.F.W acknowledges support from the Royal Academy of Engineering. J.D.M. acknowledges financial support from the Engineering and Physical Sciences Research Council (EPSRC) of the United Kingdom, via the EPSRC Centre for Doctoral Training in Metamaterials (Grant No. EP/L015331/1). S.R. and M.F.C. acknowledge financial support from EPSRC (Grant no. EP/K010050/1, EP/M001024/1, EP/M002438/1), from Royal Society international Exchanges Scheme 2016/R1, from The Leverhulme trust (grant title “Quantum Revolution” and "Quantum Drums"). A.P Rooney and S.J Haigh acknowledge support from the EPSRC postdoctoral fellowship and from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement ERC-2016-STG-EvoluTEM-715502) and the Defence Threat Reduction Agency (HDTRA1-12-1-0013). I.A. acknowledges financial support from The European Commission Marie Curie Individual Fellowships (Grant number 701704)