Strain-Engineering Induced Anisotropic Crystallite Orientation and Maximized Carrier Mobility for High-Performance Microfiber-Based Organic Bioelectronic Devices

Despite the importance of carrier mobility, recent research efforts have been mainly focused on the improvement of volumetric capacitance in order to maximize the figure-of-merit, mu C* (product of carrier mobility and volumetric capacitance), for high-performance organic electrochemical transistors. Herein, high-performance microfiber-based organic electrochemical transistors with unprecedentedly large mu C* using highly ordered crystalline poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) microfibers with very high carrier mobilities are reported. The strain engineering via uniaxial tension is employed in combination with solvent-mediated crystallization in the course of drying coagulated fibers, resulting in the permanent preferential alignment of crystalline PEDOT:PSS domains along the fiber direction, which is verified by atomic force microscopy and transmission wide-angle X-ray scattering. The resultant strain-engineered microfibers exhibit very high carrier mobility (12.9 cm(2) V-1 s(-1)) without the trade-off in volumetric capacitance (122 F cm(-3)) and hole density (5.8 x 10(20) cm(-3)). Such advantageous electrical and electrochemical characteristics offer the benchmark parameter of mu C* over approximate to 1500 F cm(-1) V-1 s(-1), which is the highest metric ever reported in the literature and can be beneficial for realizing a new class of substrate-free fibrillar and/or textile bioelectronics in the configuration of electrochemical transistors and/or electrochemical ion pumps.

Automated summary

This study reports high-performance microfiber-based organic electrochemical transistors with unprecedentedly large muC*, achieved by using highly ordered crystalline PEDOT:PSS microfibers with very high carrier mobilities. The strain engineering and solvent-mediated crystallization techniques led to the permanent preferential alignment of crystalline PEDOT:PSS domains, resulting in high carrier mobility without compromising volumetric capacitance and hole density. The advantageous electrical and electrochemical characteristics offer a benchmark parameter of mu C* over approximately 1500 F cm(-1) V-1 s(-1), which is the highest metric reported in the literature and can be beneficial for realizing a new class of substrate-free bioelectronics.