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Dryad

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

Abstract

Understanding structural and dynamic properties of inherently 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 electrolyte. 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 mesoscale strain and structural hysteresis that depend on the sample's cycling history, establishing a comprehensive kinetic sequence bridging the macroscopic and microscopic behaviors of OMIECs. Furthermore, we uncover 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.