ABSTRACT
Redox reactions of the Li+ insertion/extraction from one to two interlayers of graphene (Gr) on area-defined single-crystalline SiC substrates are investigated using lithium phosphorus oxynitride glass (LiPON) as the solid-state electrolyte. Unlike an organic liquid electrolyte, this glassy electrolyte does not induce a reduction current and excludes the desolvation reaction of Li+. Gr electrodes with less than two Gr layers show a single reduction peak and one or two oxidation peaks below +0.21 V (vs Li+/Li), differing distinctly from those of graphite and multilayer Gr, which display multiple peaks (multiple stage transitions). However, this finding aligns with the conventional understanding that graphite stage structure transitions proceed with stepwise increases or decreases in the number of Gr layers between adjacent Li-inserted interlayers. Cyclic voltammetry measurements indicate the presence of surface capacity due to Li+ adsorption/desorption at the LiPON/Gr interface. Moreover, Li+ insertion and extraction induce different charge transfer resistances at the level of a single interlayer. These sensitive measurements are achieved using high-quality epitaxial Gr and LiPON electrolyte, which prevent the formation of a solid electrolyte interphase and the desolvation reaction of Li+. Similar measurements using bilayer Gr produced by chemical vapor deposition coupled with a Gr transfer method and an ethylene carbonate/dimethyl carbonate liquid electrolyte are not reliable. Thus, the proposed method is effective for electrochemical measurement of Gr electrodes with a controlled number of layers.
ABSTRACT
Graphene on SiC (0001â¾) tends to grow in multiple layers and does not have a single orientation relation with the SiC substrate. It has been considered impossible to control the rotation angle of multilayer graphene on SiC (0001â¾). In this study, we grew graphene on off-axis SiC substrates with various off angles from 0° to 8° and investigated their in-plane rotation and electronic structures systematically. As the off angle toward the [112â¾0]SiCdirection increased, graphene rotated by 30° with respect to SiC became less dominant and instead, graphene rotated by 30 ± 2.5° appeared. We also found that the uniformity of the graphene rotation angle was relatively high on SiC substrates with a small off angle toward the [11â¾00]SiCdirection. Our results suggest that the step-terrace structure defined by the substrate off-direction and angle plays an important role in the controllability of the rotation angle of graphene.
