The residue of common photo‐ and electron‐beam resists, such as poly(methyl methacrylate) (PMMA), is often present on the surface of 2D crystals after device fabrication. The residue degrades device properties by decreasing carrier mobility and creating unwanted doping. Here, MoS2 and WSe2 field effect transistors (FETs) with residue are cleaned by contact mode atomic force microscopy (AFM) and the impact of the residue on: 1) the intrinsic electrical properties, and 2) the effectiveness of electric double layer (EDL) gating are measured. After cleaning, AFM measurements confirm that the surface roughness decreases to its intrinsic state (i.e., ≈0.23 nm for exfoliated MoS2 and WSe2) and Raman spectroscopy shows that the characteristic peak intensities (E2g and A1g) increase. PMMA residue causes p‐type doping corresponding to a charge density of ≈7 × 1011 cm−2 on back‐gated MoS2 and WSe2 FETs. For FETs gated with polyethylene oxide (PEO)76:CsClO4, removing the residue increases the charge density by 4.5 × 1012 cm−2, and the maximum drain current by 247% (statistically significant, p < 0.05). Removing the residue likely allows the ions to be positioned closer to the channel surface, which is essential for achieving the best possible electrostatic gate control in ion‐gated devices.
Electric double-layer (EDL) gating using a custom-synthesized polyester single-ion conductor (PE400-Li) is demonstrated on two-dimensional (2D) crystals for the first time. The electronic properties of graphene and MoTe2 field-effect transistors (FETs) gated with the single-ion conductor are directly compared to a poly(ethylene oxide) dual-ion conductor (PEO:CsClO4). The anions in the single-ion conductor are covalently bound to the backbone of the polymer, leaving only the cations free to form an EDL at the negative electrode and a corresponding cationic depletion layer at the positive electrode. Because the cations are mobile in both the single- and dual-ion conductors, a similar enhancement of the n-branch is observed in both graphene and MoTe2. Specifically, the single-ion conductor decreases the subthreshold swing in the n-branch of the bare MoTe2 FET from 5000 to 250 mV/dec and increases the current density and on/off ratio by two orders of magnitude. However, the single-ion conductor suppressed the p-branch in both the graphene and the MoTe2 FETs, and finite element modeling of ion transport shows that this result is unique to single-ion conductor gating in combination with an asymmetric gate/channel geometry. Both the experiments and modeling suggest that single-ion conductor-gated FETs can achieve sheet densities up to 1014 cm–2, which corresponds to a charge density that would theoretically be sufficient to induce several percent strain in monolayer 2D crystals and potentially induce a semiconductor-to-metal phase transition in MoTe2.
A gateless lateral p-n junction with reconfigurability is demonstrated on graphene by ion-locking using solid polymer electrolytes. Ions in the electrolytes are used to configure electric-double-layers (EDLs) that induce pand n-type regions in graphene. These EDLs are locked in place by two different electrolytes with distinct mechanisms: (1) a polyethylene oxide (PEO)-based electrolyte, PEO:CsClO 4 , is locked by thermal quenching (i.e., operating temperature < T g (glass transition temperature)), and (2) a custom-synthesized, doubly-polymerizable ionic liquid (DPIL) is locked by thermally triggered polymerization that enables room temperature operation. Both approaches are gateless because only the source/drain terminals are required to create the junction, and both show two current minima in the backgated transfer measurements, which is a signature of a graphene p-n junction. The PEO:CsClO 4 gated p-n junction is reconfigured to n-p by resetting the device at room temperature, reprogramming, and cooling to T < T g . These results show an alternate approach to locking EDLs on 2D devices and suggest a path forward to reconfigurable, gateless lateral p-n junctions with potential applications in polymorphic logic circuits.
Controlling the mobile ion content of ioncontaining polymers is critical for advanced organic electronic applications. Here, we report a chemical strategy for achieving "on-demand" release of ions in polymeric materials by incorporating thermally labile Diels−Alder linkages into polymerized ionic liquids. Electrical characterization demonstrates a clear increase in mobile ion content at the retro-Diels−Alder temperature, which is retained after the material is returned to room temperature. This work demonstrates that chemical triggers can be utilized to release ions and change the mobile ion content of a polymeric material after the sample is prepared, paving the way for new classes of responsive organic electronic devices.
A molecularly thin electrolyte is developed to demonstrate a nonvolatile, solid-state, one-transistor (1T) memory based on an electric-double-layer (EDL) gated WSe2 field-effect transistor (FET). The custom-designed monolayer electrolyte consists of cobalt crown ether phthalocyanine and lithium ions, which are positioned by field-effect at either the surface of the WSe2 channel or an h-BN capping layer to achieve “1” or “0”, respectively. Bistability in the monolayer electrolyte memory is significantly improved by the h-BN cap with density functional theory (DFT) calculations showing enhanced trapping of Li+ near h-BN due to a ∼1.34 eV increase in the absolute value of the adsorption energy compared to vacuum. The threshold voltage shift between the two states corresponds to a change in charge density of ∼2.5 × 1012 cm–2, and an On/Off ratio exceeding 104 at a back gate voltage of 0 V. The On/Off ratio remains stable after 1000 cycles and the retention time for each state exceeds 6 h (max measured). When the write time approaches 1 ms, the On/Off ratio remains >102, showing that the monolayer electrolyte-gated FET can respond on time scales similar to existing flash memory. The data suggest that faster switching times and lower switching voltages could be feasible by top gating.
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