Impact of Water-Water Correlation at Suspended Graphene/Water Interface Under Different Electro-Modulated
Authors: LU Yuxuan , Lin Fang-Min , Long Wei-Yu , Lin Chih-Ting 
Published: August 2024

Graphene-based devices have extensive applications in aqueous environments. The molecular interactions across the graphene sheet significantly impact various devices, although few researches focused on elucidating the interface effects. In this study, we utilize trench structure to make graphene unilaterally and bilaterally suspended in water. The conduction status of both lateral and longitudinal currents (Id, Is, Ig) of graphene was monitored under two suspension scenarios to investigate the changes in interface evolution with the introduction of solvent-solvent interactions. For unilaterally suspended graphene, the current perpendicular to the graphene channel direction remains in the off state. For bilaterally suspended graphene, the current path is formed vertically between the graphene channel and the gate electrode, perpendicular to the direction of the graphene. This experimental setup illustrates the possibilities for exploring interfacial characteristics at the interface between 2D materials and solutions through practical experimentation.
The detailed fabrication process of the graphene field-effect-transistor (GFET) device is depicted in Fig. 1. To fabricate the microchannel structure, a microfluidic pattern was generated through photolithography on the SiO2/Si substrate spun with a layer of photoresist. Then, the corresponding microchannel pattern with a thickness of 300 nm SiO2 and 30 μm Si layer was etched by reactive-ion etching (RIE) to form a trench capable of storing water. Afterward, Au electrodes were placed next to the microfluidic channel via evaporation utilizing a shadow mask. The second critical step involves the preparation of graphene. Graphene sheets were grown on a copper foil through the chemical vapor deposition (CVD) method. With the support of PMMA film, physically stacked graphene bilayer graphene was transferred to the target substrate. Ultimately, the suspended bilayer graphene was submerged in acetone for 24 hours to remove the PMMA layer and immersed in isopropanol (IPA) and DI water to clean the residues.
According to this device structure, we successfully fabricate the suspension of graphene unilaterally or bilaterally in water. When introducing water through the trench, the bottom surface of the suspended graphene contacts with water molecules, while the upper surface of the suspended graphene is exposed to air. This configuration leads to a unilateral suspension in water (unilateral-suspension GFET). Conversely, when water is introduced through the trench and water is also added above the graphene channel, graphene comes into contact with water on both sides. This configuration results in its bilateral suspension in the water (bilateral-suspension GFET). The electronic transport characteristics of unilateral-suspension GFET and bilateral-suspension GFET were measured by Agilent semiconductor analysis B1500A. The gate voltage was applied to water through an Ag/AgCl electrode. Fig. 2 (a) displays the Raman spectroscopy of suspended graphene on GFET device. The most notable features of the Raman spectrum are the G peak around 1580 cm-1, and the 2D band around 2700 cm-1, which are typical characteristics of graphene. The ID/IG ratio of 0.19 indicates the good quality of the graphene layers. As shown in Fig. 2 (b), the scanning electron microscope (SEM) result of suspended graphene on the GFET device verifies the presence of large-area graphene. The diagram displays a clear demarcation line, facilitating the identification of graphene presence on the substrate. This can also imply the excellent quality of graphene with few defects.
The transport behavior of unilateral-suspension GFET and bilateral-suspension GFET are measured individually, as shown in Fig. 3. The sum (ΔI) of The drain current behavior (Id) and source current behavior (Is), and gate current behavior (Ig) are recorded with changed gate voltages (from -1V to +1V) and constant VDS (VDS= 0.1V). For unilateral-suspension GFET, ΔI and Ig keep constant at zero, and there is no conduction path perpendicular to the graphene channel direction. For bilateral-suspension GFET, ΔI and Ig at positive gate voltage are opposite in direction and equal in absolute value, this indicates the formation of an obvious path between the channel and gate electrode. The apparent interfacial evolution is believed to change with the introduction of the other side of water.
In conclusion, we compare the electrical characteristics shown by two different suspension situations of graphene-based field effect transistors. There are some interesting results of the conduction path relating to interfacial evolution. This result has potential for chemical sensing or battery application. Furthermore, it can contribute to fundamental research about the interface interaction between suspended graphene and water.

Figure 1