Increasing the Room-Temperature Electric Double Layer Retention Time in Two-Dimensional Crystal FETs

Poly(vinyl alcohol) (PVA) and LiClO₄, a solid polymer electrolyte with a glass transition temperature (T_g) of 80 °C, is used to electrostatically gate graphene field-effect transistors. The ions in PVA:LiClO₄ are drifted into place by field-effect at T > T_g, providing n- or p-type doping, and when the device is cooled to room temperature, the polymer mobility and, hence ion mobility are arrested and the electric double layer (EDL) is "locked" into place in the absence of a gate bias. Unlike other electrolytes used to gate two-dimensional devices for which the T_g, and therefore the "locking" temperature, is well below room temperature, the electrolyte demonstrated in this work provides a route to achieve room-temperature EDL stability. Specifically, a 6 orders of magnitude increase in the room temperature EDL retention time is demonstrated over the commonly used electrolyte, poly(ethylene oxide) (PEO) and LiClO₄. Hall measurements confirm that large sheet carrier densities can be achieved with PVA:LiClO₄ at top gate programming voltages of ±2 V (-6.3 ± 0.03 × 10¹³ cm^-2 for electrons and 1.6 ± 0.3 × 10¹⁴ cm^-2 for holes). Transient drain current measurements show that at least 75% of the EDL is retained after more than 4 h at room temperature. Unlike PEO-based electrolytes, PVA:LiClO₄ is compatible with the chemicals used in standard photolithographic processes enabling the direct deposition of patterned, metal contacts on the surface of the electrolyte. A thermal instability in the electrolyte is detected by both I-V measurements and differential scanning calorimetry, and FTIR measurements suggest that thermally catalyzed cross-linking may be driving phase separation between the polymer and the salt. Nevertheless, this work highlights how the relationship between polymer and ion mobility can be exploited to tune the state retention time and the charge carrier density of a 2D crystal transistor.