Abstract

AbstractTwo new glycolated semiconducting polymers PgBT(F)2gT and PgBT(F)2gTT of differing backbone curvatures were designed and synthesised for application as p‐type accumulation mode organic electrochemical transistor (OECT) materials. Both polymers demonstrated stable and reversible oxidation, accessible within the aqueous electrochemical window, to generate polaronic charge carriers. OECTs fabricated from PgBT(F)2gT featuring a curved backbone geometry attained a higher volumetric capacitance of 170 F cm−3. However, PgBT(F)2gTT with a linear backbone displayed overall superior OECT performance with a normalised peak transconductance of 3.00×104 mS cm−1, owing to its enhanced order, expediting the charge mobility to 0.931 cm2 V−1 s−1.

Highlights

  • Two new glycolated semiconducting polymers PgBT(F)2gT and PgBT(F)2gTT of differing backbone curvatures were designed and synthesised for application as p-type accumulation mode organic electrochemical transistor (OECT) materials

  • Developments in OECT polymer designs have progressed towards donor–acceptor (D–A) conjugated backbones.[16,17,18,19]

  • Refined energy level tuning is an important advantage of applying D–A backbones, which can be exploited to improve electrochemical/OECT stability by avoidance of undesirable redox side-reactions,[20,21] as well as to ensure OECT operation in favourable accumulation mode, where channel conductivity is negligible at resting gate potential, and grows with increased gate bias (c.f. depletion mode with vice versa operational characteristics).[22]

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Summary

Chemie applying an oxidative potential of

0.4 V vs. Ag/AgCl, which was incremented up to 0.8 V, gradual quenching of the PgBT(F)2gT ground state transitions was observed, concurrent with the appearance and intensification of a broad polaron band at 850 nm. UV/Vis spectrum, evidencing electrochemical reversibility (Figure S46). SEC of PgBT(F)2gTT thin films (Figure S47), a broad polaron band UV/Vis SEC confirms reversible generation of mobile charge carrying hole polarons on PgBT(F)2gT and PgBT(F)2gTT by electrochemical oxidation. The p-type accumulation mode OECT performance of and square-wave voltammetry (SQW) electrochemical data devices fabricated using PgBT(F)2gT and PgBT(F)2gTT were in 0.1 M KCl/H2O (Figure 2), the onset of PgBT(F)2gT thin film oxidation occurs at 0.4 V vs Ag/AgCl (HOMO = À4.8 eV[38]), which lies well within the aqueous electrochemical window but sufficiently anodic to avoid material ambient interpreted using the transconductance expression [Eq (1),. Cycling CV experiments suggested excellent electrochemical stability and reversibility of PgBT(F)2gT gm 1⁄4

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