Pulse Dynamics of Electric Double Layer Formation on All-Solid-State Graphene Field-Effect Transistors.

Electric double layer (EDL) dynamics in graphene field-effect transistors (FETs) gated with polyethylene oxide (PEO)-based electrolytes are studied by molecular dynamics (MD) simulations from picoseconds to nanoseconds and experimentally from microseconds to milliseconds. Under an applied field of approximately mV/nm, EDL formation on graphene FETs gated with PEO:CsClO occurs on the timescale of microseconds at room temperature and strengthens within 1 ms to a sheet carrier density of n ≈ 10 cm. Stronger EDLs (i.e., larger n) are induced experimentally by pulsing with applied voltages exceeding the electrochemical window of the electrolyte; electrochemistry is avoided using short pulses of a few milliseconds. Dynamics on picosecond to nanosecond timescales are accessed using MD simulations of PEO:LiClO between graphene electrodes with field strengths of hundreds of mV/nm which is 100× larger than experiment. At 100 mV/nm, EDL formation initiates in sub-nanoseconds achieving charge densities up to 6 × 10 cm within 3 nanoseconds. The modeling shows that under sufficiently high electric fields, EDLs with densities ∼10 cm can form within a nanosecond, which is a timescale relevant for high-performance electronics such as EDL transistors (EDLTs). Moreover, the combination of experiment and modeling shows that the timescale for EDL formation ( n = 10 to 10 cm) can be tuned by 9 orders of magnitude by adjusting the field strength by only 3 orders of magnitude.