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Tang, Qizhe ; Barwick, Isabelle ; Han, Qi ; Watts, Benjamin ; Thomsen, Lars ; Hungenberg, Julian ; Gebert, Matthew ; Eller, Fabian ; Herzig, Eva M. ; Thelakkat, Mukundan ; Guo, Keying ; McNeill, Christopher R.:
Tuning Mixed Conduction between Ionic and Electronic Transport in Blended OMIECs via Phase Separation and Selective Dissolution.
In: ACS Applied Materials & Interfaces.
(20 Mai 2026)
.
ISSN 1944-8252
DOI: https://doi.org/10.1021/acsami.6c05714
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| Projekttitel: |
Offizieller Projekttitel Projekt-ID GRK 2818: Optische Anregungen in organischen und anorganischen Halbleitern: Verstehen und Kontrollieren durch externe Stimuli 464648186 |
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Deutsche Forschungsgemeinschaft |
Abstract
This study reveals how the morphology of organic mixed ionic-electronic conductors (OMIECs) controls the mixed ionic-electronic transport of organic electrochemical transistors (OECTs). Two p-type OMIECs with oligoethylene glycol (OEG) side chains, namely P3MEEET and P3MEEMT, are blended with polystyrene (PS) to produce laterally phase-separated morphologies. By varying the ratio between OMIEC and PS, distinct morphologies are created via nucleation and growth and via spinodal decomposition. Furthermore, porous films are fabricated through the selective dissolution of PS, providing a direct comparison between blend and porous structures on OECT performance. In blends, the reduced ion injection area significantly enhances the mobility (μ) and figure of merit (μC*). Due to the hydrophilic nature of the OMIECs, adding pores to the films does not have a positive effect on signal amplification but improves ion storage via side injection and increases the effective volumetric capacitance (C*). Comparing the two OMIECs studied, porous samples based on P3MEEMT experience a greater benefit from electrolyte side injection. Both blend and porous samples are characterized using a range of techniques, including spectroelectrochemistry (SEC), atomic force microscopy (AFM), scanning transmission X-ray microscopy (STXM), quartz crystal microbalance (QCM), along with ex situ and in situ grazing-incidence wide-angle X-ray scattering (GIWAXS) to unravel the mechanism of the mixed ionic-electronic transport from both an ionic and electronic perspective.This study reveals how the morphology of organic mixed ionic-electronic conductors (OMIECs) controls the mixed ionic-electronic transport of organic electrochemical transistors (OECTs). Two p-type OMIECs with oligoethylene glycol (OEG) side chains, namely P3MEEET and P3MEEMT, are blended with polystyrene (PS) to produce laterally phase-separated morphologies. By varying the ratio between OMIEC and PS, distinct morphologies are created via nucleation and growth and via spinodal decomposition. Furthermore, porous films are fabricated through the selective dissolution of PS, providing a direct comparison between blend and porous structures on OECT performance. In blends, the reduced ion injection area significantly enhances the mobility (μ) and figure of merit (μC*). Due to the hydrophilic nature of the OMIECs, adding pores to the films does not have a positive effect on signal amplification but improves ion storage via side injection and increases the effective volumetric capacitance (C*). Comparing the two OMIECs studied, porous samples based on P3MEEMT experience a greater benefit from electrolyte side injection. Both blend and porous samples are characterized using a range of techniques, including spectroelectrochemistry (SEC), atomic force microscopy (AFM), scanning transmission X-ray microscopy (STXM), quartz crystal microbalance (QCM), along with ex situ and in situ grazing-incidence wide-angle X-ray scattering (GIWAXS) to unravel the mechanism of the mixed ionic-electronic transport from both an ionic and electronic perspective.