Qiongyu Li

Millimeter-Size Single-Crystal Graphene by Suppressing Evaporative Loss of Cu During Low Pressure Chemical Vapor Deposition

Millimeter-size single-crystal monolayer graphene is synthesized on polycrystalline Cu foil by a method that involves suppressing loss by evaporation of the Cu at high temperature under low pressure. This significantly diminishes the number of graphene domains, and large single crystal domains up to ∼2 mm in size are grown.

Quantitative correlation between defect density and heterogeneous electron transfer rate of single layer graphene

Improving electrochemical activity of graphene is crucial for its various applications, which requires delicate control over its geometric and electronic structures. We demonstrate that precise control of the density of vacancy defects, introduced by Ar(+) irradiation, can improve and finely tune the heterogeneous electron transfer (HET) rate of graphene. For reliable comparisons, we made patterns with different defect densities on a same single layer graphene sheet, which allows us to correlate defect density (via Raman spectroscopy) with HET rate (via scanning electrochemical microscopy) of graphene quantitatively, under exactly the same experimental conditions. By balancing the defect induced increase of density of states (DOS) and decrease of conductivity, the optimal HET rate is attained at a moderate defect density, which is in a critical state; that is, the whole graphene sheet becomes electronically activated and, meanwhile, maintains structural integrity. The improved electrochemical activity can be understood by a high DOS near the Fermi level of defective graphene, as revealed by ab initio simulation, which enlarges the overlap between the electronic states of graphene and the redox couple. The results are valuable to promote the performance of graphene-based electrochemical devices. Furthermore, our findings may serve as a guide to tailor the structure and properties of graphene and other ultrathin two-dimensional materials through defect density engineering.

Thermal conductivity measurements of suspended graphene with and without wrinkles by micro-Raman mapping

The thermal conductivity (κ) of suspended graphene membranes made by chemical vapor deposition (CVD) was measured by micro-Raman mapping. Cracks and wrinkles present in these suspended graphene membranes were identified by micro-Raman mapping, and κ values and their statistics were obtained on membranes free of such imperfections in a single mapping. Based on this new technique, an average κ value of 1875 ± 220 W m(-1) K(-1) at 420 K was measured on 26 suspended graphene membranes that were free of wrinkles, ~27% higher than the average value measured from 12 graphene membranes with wrinkles. These results suggest that the variation in published thermal conductivity values for suspended graphene samples could, at least in part, be due to the presence or absence of wrinkles.

Graphene-Based Fluorescence-Quenching-Related Fermi Level Elevation and Electron-Concentration Surge

Intermolecular p-orbital overlaps in unsaturated π-conjugated systems, such as graphene and fluorescent molecules with aromatic structure, serve as the electron-exchanged path. Using Raman-mapping measurements, we observe that the fluorescence intensity of fluorescein isothiocyanate (FITC) is quenched by graphene, whereas it persists in graphene-absent substrates (SiO2). After identifying a mechanism related to photon-induced electron transfer (PET) that contributes to this fluorescence quenching phenomenon, we validate this mechanism by conducting analyses on Dirac point shifts of FITC-coated graphene. From these shifts, Fermi level elevation and the electron-concentration surge in graphene upon visible-light impingements are acquired. Finally, according to this mechanism, graphene-based biosensors are fabricated to show the sensing capability of measuring fluorescently labeled-biomolecule concentrations.