Engineering Graphene Conductivity for Flexible and High-Frequency Applications

Advances in lightweight, flexible, and conformal electronic devices depend on materials that exhibit high electrical conductivity coupled with high mechanical strength. Defect-free graphene is one such material that satisfies both these requirements and which offers a range of attractive and tunable electrical, optoelectronic, and plasmonic characteristics for devices that operate at microwave, terahertz, infrared, or optical frequencies. Essential to the future success of such devices is therefore the ability to control the frequency-dependent conductivity of graphene. Looking to accelerate the development of high-frequency applications of graphene, here we demonstrate how readily accessible and processable organic and organometallic molecules can efficiently dope graphene to carrier densities in excess of 10(13) cm(-2) with conductivities at gigahertz frequencies in excess of 60 mS. In using the molecule 3,6-difluoro-2,5,7,7,8,8-hexacyanoquinodirnethane (F2-HCNQ), a high charge transfer (CT) of 0.5 electrons per adsorbed molecule is calculated, resulting in p-type doping of graphene. n-Type doping is achieved using cobaltocene and the sulfur-containing molecule tetrathiafulvalene (TTF) with a CT of 0.41 and 0.24 electrons donated per adsorbed molecule, respectively. Efficient CT is associated with the interaction between the pi electrons present in the molecule and in graphene. Calculation of the high-frequency conductivity shows dispersion-less behavior of the real component of the conductivity over a wide range of gigahertz frequencies. Potential high-frequency applications in graphene antennas and communications that can exploit these properties and the broader impacts of using molecular doping to modify functional materials that possess a low-energy Dirac cone are also discussed.