Alkyl chain length-engineered electric double layer for enhanced thermoelectric modulation in SWCNTs via ionic liquid gating
摘要
Ionic gating offers a highly reversible and precise means to modulate the thermoelectric (TE) properties of low-dimensional semiconductors. However, how the molecular structure of electrolytes affects the efficiency of such modulation remains poorly understood. In this work, we constructed organic electrochemical transistors (OECTs) based on single-walled carbon nanotubes (SWCNTs) to investigate thermoelectric modulation via ionic gating. Two imidazolium-based ionic liquids, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM][TFSI]) and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BMIM][TFSI]), were employed to examine the influence of cation structure on electric double layer configuration and the resulting modulated effects on thermoelectric response of both the p- and n-type. Notably, the [BMIM][TFSI] system facilitated an earlier transition from p- to n-type conduction at relatively low gate voltages (VG), with the n-type region exhibiting strong TE responsiveness, indicating enhanced carrier tunability. Molecular dynamics (MD) simulations further revealed that variations in ionic liquid molecular structure influenced the electric double layer (EDL) strength, thereby affecting carrier transport characteristics. This study offers both experimental and theoretical insights into the structure–property relationship of ionic gating systems, and provides a viable strategy for designing high-performance, gate-tunable TE devices.