Role of aggregates and microstructure of mixed-ionic–electronic-conductors on charge transport in electrochemical transistors

LeCroy, Garrett; Cendra, Camila; Quill, Tyler J.; Moser, Maximilian; Hallani, Rawad; Ponder, Jr., James F.; Stone, Kevin; Kang, Stephen D.; Liang, Allen Yu-Lun; Thiburce, Quentin; McCulloch, Iain; Spano, Frank C.; Giovannitti, Alexander; Salleo, Alberto

doi:10.1039/d3mh00017f

Title: Role of aggregates and microstructure of mixed-ionic–electronic-conductors on charge transport in electrochemical transistors

Journal Article · 24 April 2023 · Materials Horizons

DOI: https://doi.org/10.1039/d3mh00017f · OSTI ID:1995727

^[1]; Cendra, Camila ^[1]; Quill, Tyler J. ^[1];

^[2]; Hallani, Rawad ^[3]; Ponder, Jr., James F. ^[4];

^[5]; Kang, Stephen D. ^[1];

^[1]; Thiburce, Quentin ^[1]; McCulloch, Iain ^[6]; Spano, Frank C. ^[7];

^[8]; Salleo, Alberto ^[1]

Stanford Univ., CA (United States)
Univ. of Oxford (United Kingdom)
King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States); UES, Inc., Dayton, OH (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Univ. of Oxford (United Kingdom); King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Temple Univ., Philadelphia, PA (United States)
Stanford Univ., CA (United States); Chalmers University of Technology, Gothenburg (Sweden)

Synthetic efforts have delivered a library of organic mixed ionic–electronic conductors (OMIECs) with high performance in electrochemical transistors. The most promising materials are redox-active conjugated polymers with hydrophilic side chains that reach high transconductances in aqueous electrolytes due to volumetric electrochemical charging. Current approaches to improve transconductance and device stability focus mostly on materials chemistry including backbone and side chain design. However, other parameters such as the initial microstructure and microstructural rearrangements during electrochemical charging are equally important and are influenced by backbone and side chain chemistry. In this study, we employ a polymer system to investigate the fundamental electrochemical charging mechanisms of OMIECs. We couple in situ electronic charge transport measurements and spectroelectrochemistry with ex situ X-ray scattering electrochemical charging experiments and find that polymer chains planarize during electrochemical charging. Our work shows that the most effective conductivity modulation is related to electrochemical accessibility of well-ordered, interconnected aggregates that host high mobility electronic charge carriers. Electrochemical stress cycling induces microstructural changes, but we find that these aggregates can largely maintain order, providing insights on the structural stability and reversibility of electrochemical charging in these systems. Finally, this work shows the importance of material design for creating OMIECs that undergo structural rearrangements to accommodate ions and electronic charge carriers during which percolating networks are formed for efficient electronic charge transport.

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Research Organization:: Stanford Univ., CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE

Contributing Organization:: University of Oxford

Grant/Contract Number:: AC02-76SF00515; DMR 1808401; SC0020046; DGE-1656518; ECCS-1542152; SC0014664

OSTI ID:: 1995727

Alternate ID(s):: OSTI ID: 1971262

Journal Information:: Materials Horizons, Vol. 10, Issue 7; ISSN 2051-6347

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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