Control of growth kinetics during remote epitaxy of complex oxides on graphene by pulsed laser deposition

Remote epitaxy through 2D materials opens new opportunities for research and application, overcoming some limitations of classical epitaxy and allowing the creation of freestanding layers. However, using graphene as a 2D interlayer for remote epitaxy of metal oxides is challenging, particularly when carried out by pulsed laser deposition (PLD). The graphene layer can be easily oxidized under the typically applied high oxygen pressures, and the impact of highly kinetic particles of the plasma plume can lead to severe damages. In this study, both aspects are addressed: Argon is introduced as an inert background gas in order to avoid oxidation and to reduce the kinetic impact of the plasma species on graphene. The laser spot size is minimized to control the plasma plume and particle flux. As a model system, strontium titanate (STO) is quasi-homoepitaxially grown on graphene buffered STO single crystals. Raman spectroscopy is performed to evaluate the 2D, G, and D band fingerprints of the graphene layer and to assess the defect structure of the interlayer after the deposition. Our results prove that control of the growth kinetics by reducing the laser spot size and by using high argon pressures provides a key strategy to conserve graphene with a low defect density during PLD while allowing a layer-by-layer growth of structurally coherent oxide layers. This strategy may be generalized for the PLD remote epitaxy of many complex oxides, opening the way for integrating 2D materials with complex oxides using widely accessible PLD processes.