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 (Tg) 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 > Tg, 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 Tg, 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.

Monolayer Solid-State Electrolyte for Electric Double Layer Gating of Graphene Field-Effect Transistors.

The electrostatic gating of graphene field-effect transistors is demonstrated using a monolayer electrolyte. The electrolyte, cobalt crown ether phthalocyanine (CoCrPc) and LiClO4, is deposited as a monolayer on the graphene channel, essentially creating an additional two-dimensional layer on top of graphene. The crown ethers on the CoCrPc solvate lithium ions and the ion location is modulated by a backgate without requiring liquid solvent. Ions dope the channel by inducing image charges; the doping level (i.e., induced charge density) can be modulated by the backgate bias with the extent of the surface potential change being controlled by the magnitude and polarity of the backgate bias. With a crown ether to Li+ ratio of 5:1, programming tests for which the backgate is held at -VBG shift the Dirac point by ∼15 V, corresponding to a sheet carrier density on the order of 1012 cm-2. This charge carrier density agrees with the packing density of monolayer CoCrPc on graphene that would be expected with one Li+ for every five crown ethers (at the maximum possible Li+ concentration, 1013 cm-2 is predicted). The crown ethers provide two stable states for the Li+: one near the graphene channel (low-resistance state) and one ∼5 Å away from the channel (high-resistance state). Initial state retention measurements indicate that the two states can be maintained for at least 30 min (maximum time monitored), which is 106 times longer than polymer-based electrolytes at room temperature, with at least a 250 Ω µm difference between the channel resistance in the high- and low-resistance states.

Reconfigurable Ion Gating of 2H-MoTe2 Field-Effect Transistors Using Poly(ethylene oxide)-CsClO4 Solid Polymer Electrolyte.

Transition metal dichalcogenides are relevant for electronic devices owing to their sizable band gaps and absence of dangling bonds on their surfaces. For device development, a controllable method for doping these materials is essential. In this paper, we demonstrate an electrostatic gating method using a solid polymer electrolyte, poly(ethylene oxide) and CsClO4, on exfoliated, multilayer 2H-MoTe2. The electrolyte enables the device to be efficiently reconfigured between n- and p-channel operation with ON/OFF ratios of approximately 5 decades. Sheet carrier densities as high as 1.6 × 10(13) cm(-2) can be achieved because of a large electric double layer capacitance (measured as 4 µF/cm(2)). Further, we show that an in-plane electric field can be used to establish a cation/anion transition region between source and drain, forming a p-n junction in the 2H-MoTe2 channel. This junction is locked in place by decreasing the temperature of the device below the glass transition temperature of the electrolyte. The ideality factor of the p-n junction is 2.3, suggesting that the junction is recombination dominated.