Self-assembled organic layers containing various functional groups between graphene layers were examined as gas barrier films. The formation of well-defined self-assembled layers of functionalized alkane molecules on graphene was confirmed by scanning tunneling microscopy (STM). The roles of these organic layers as gas barrier films could be quantitatively deduced by comparing their water vapor transmission rate (WVTR). The formation of self-assembled layers dramatically improved gas barrier properties by primarily blocking defects and gas molecule pathways. For functionalized alkanes containing hydrophilic groups, more enhanced gas barrier properties were observed compared to those with hydrophobic groups. These results clearly indicate that the primary role of the organic layers in gas barrier films is to block defects and the pathways of water molecules, with a secondary role of delaying the movement of water molecules through hydrogen bonding interactions.

In this study, laser-induced graphene oxide (LIGO) was synthesized through a facile liquid-based process involving the introduction of deionized (DI) water onto polyimide (PI) film and subsequent direct laser irradiation using a CO2 laser (λ = 10.6 μm). The synthesized LIGO was then evaluated as a sensing material for monitoring changes in humidity levels. The synthesis conditions were optimized by precisely controlling the laser scribing speed, leading to the synthesis of LIGO with different structural characteristics and varying oxygen contents. The increased number of oxygen-containing functional groups contributed to the hydrophilic properties of LIGO, resulting in a superior humidity sensing capabilities compared with laser-induced graphene (LIG). The LIGO-based sensors outperformed LIG-based sensors, demonstrating approximately tenfold higher sensing responsivity when detecting changes at each humidity level, along with 1.25 to 1.75 times faster response/recovery times, making LIGO-based sensors more promising for humidity-monitoring applications. This study demonstrated laser ablation in a renewable and natural precursor as an eco-friendly and energy-efficient approach to directly synthesize LIGO with controllable oxidation levels.