A detailed description of the electronic properties, chemical state, and structure of uniform single and few-layered graphene oxide (GO) thin films at different stages of reduction is reported. The residual oxygen content and structure of GO are monitored and these chemical and structural characteristics are correlated to electronic properties of the thin films at various stages of reduction. It is found that the electrical characteristics of reduced GO do not approach those of intrinsic graphene obtained by mechanical cleaving because the material remains significantly oxidized. The residual oxygen forms sp3 bonds with carbon atoms in the basal plane such that the carbon sp2 bonding fraction in fully reduced GO is ca 0.80. The minority sp3 bonds disrupt the transport of carriers delocalized in the sp2 network, limiting the mobility, and conductivity of reduced GO thin films. Extrapolation of electrical conductivity data as a function of oxygen content reveals that complete removal of oxygen should lead to properties that are comparable to graphene
We elucidate the atomic and electronic structure of graphene oxide (GO) using annular dark field imaging of single and multilayer sheets and electron energy loss spectroscopy for measuring the fine structure of C and O K-edges in a scanning transmission electron microscope. Partial density of states and electronic plasma excitations are also measured for these GO sheets showing unusual π* + σ* excitation at 19 eV. The results of this detailed analysis reveal that the GO is rough with an average surface roughness of 0.6 nm and the structure is predominantly amorphous due to distortions from sp 3 C-O bonds. Around 40% sp 3 bonding was found to be present in these sheets with measured O/C ratio of 1:5. These sp 2 to sp 3 bond modifications due to oxidation are also supported by ab initio calculations.
We describe the use of single-wall carbon nanotube (SWNT) thin films as transparent and conducting electrodes for hole collection in poly(hexyl)thiophene-[6-6]phenyl-C61-butyric acid methyl ester (P3HT-PCBM) organic photovoltaics. We report a power conversion efficiency of 1%, with a fill factor of 0.3 and a short-circuit current of 6.5mA∕cm2 under 100mW∕cm2 polychromatic white light illumination measured in air. These values are comparatively higher than reference cells of similar thickness made on indium tin oxide (ITO) glass substrates. This is attributed to the three-dimensional nature of the interface between the SWNTs and the P3HT-PCBM nanocomposite. Our results indicate that solution processed SWNT thin films are a viable alternative to ITO for photovoltaic devices, eliminating an expensive vacuum deposition step in the fabrication of organic solar cells.
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