Influence of redox molecules on the electronic conductance of single-walled carbon nanotube field-effect transistors: application to chemical and biological sensing

In an effort to develop sensitive nanoscale devices for chemical and biological sensing, we have examined, using liquid gating, the conductance of semiconducting single-walled carbon nanotube-based field-effect transistors (SWCNT-FETs) in the presence of redox mediators. As examples, redox couples K3Fe(CN)6/K4Fe(CN)6 and K2IrCl6/K3IrCl6 are shown to modulate the SWCNT-FET conductance in part through their influence via the electrolyte gate on the electrostatic potential of the solution, as described by Larrimore et al. (Nano Lett. 2006, 6, 3129-1333) and in part through electron transfer between the redox mediators and the nanotubes. In the latter case, the rate of electron transfer is determined by the difference in chemical potential between the redox mediator and the SWCNTs and by the concentrations of the oxidized and reduced forms of the redox couple. Furthermore, these devices can detect the activity of redox enzymes through their sensitivity to the change in oxidation state of the enzyme substrate. An example is given for the blue copper oxidase, Trametes versicolor laccase, in which the rate of change of the SWCNT device conductance is linearly proportional to the rate of oxidation of the substrate 10-(2-hydroxyethyl)phenoxazine, varied over 2 orders of magnitude by the laccase concentration in the picomolar range. The behavior described in this work provides a highly sensitive means with which to do chemical and biological sensing using SWCNTs that is different from the amperometric, capacitive, and field-effect type sensing methods previously described in the literature for this material.