Bridging length scales in organic mixed ionic–electronic conductors through internal strain and mesoscale dynamics

Wu, Ruiheng; Meli, Dilara; Strzalka, Joseph; Narayanan, Suresh; Zhang, Qingteng; Paulsen, Bryan D.; Rivnay, Jonathan; Takacs, Christopher J.

doi:10.1038/s41563-024-01813-3

Bridging length scales in organic mixed ionic–electronic conductors through internal strain and mesoscale dynamics

Journal Article · Mon Feb 26 00:00:00 EST 2024 · Nature Materials

DOI:https://doi.org/10.1038/s41563-024-01813-3· OSTI ID:2569663

^[1]; ^[1]; ^[2]; Narayanan, Suresh ^[2]; ^[2]; ^[1]; ^[1]; ^[3]

Northwestern Univ., Evanston, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Understanding the structural and dynamic properties of disordered systems at the mesoscale is crucial. This is particularly important in organic mixed ionic-electronic conductors (OMIECs), which undergo significant and complex structural changes when operated in an electrolyte. Here, in this study, we investigate the mesoscale strain, reversibility and dynamics of a model OMIEC material under external electrochemical potential using operando X-ray photon correlation spectroscopy. Our results reveal that strain and structural hysteresis depend on the sample's cycling history, establishing a comprehensive kinetic sequence bridging the macroscopic and microscopic behaviours of OMIECs. Furthermore, we uncover the equilibrium and non-equilibrium dynamics of charge carriers and material-doping states, highlighting the unexpected coupling between charge carrier dynamics and mesoscale order. These findings advance our understanding of the structure-dynamics-function relationships in OMIECs, opening pathways for designing and engineering materials with improved performance and functionality in non-equilibrium states during device operation. Understanding mesoscale structure and dynamics in organic mixed ionic-electronic conductors is crucial. Mesoscale strain kinetics and structural hysteresis have been studied, and they uncover the coupling between charge carrier dynamics and mesoscale order in organic mixed ionic-electronic conductors.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Alfred P. Sloan Foundation; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515

OSTI ID:: 2569663

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 5 Vol. 23; ISSN 1476-4660; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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