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

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

doi:10.1038/s41563-024-01813-3

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

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

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

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. 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.

Original language	English (US)
Pages (from-to)	648-655
Number of pages	8
Journal	Nature materials
Volume	23
Issue number	5
DOIs	https://doi.org/10.1038/s41563-024-01813-3
State	Accepted/In press - 2024

Funding

J.R. gratefully acknowledges funding support from the Alfred P. Sloan Foundation (award no. FG-2019-12046). R.W., B.D.P. and J.R. acknowledge support from the National Science Foundation (grant no. NSF DMR-1751308). This work is also funded by Northwestern’s MRSEC program (NSF DMR-2308691). This work utilized the SPID facility of Northwestern University’s NUANCE Center, which is partially supported by the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the Materials Research Science and Engineering Center (NSF DMR-2308691), the State of Illinois and Northwestern University. This research used resources of the Advanced Photon Source operated by the Argonne National Laboratory supported by the US Department of Energy (DOE), Office of Science (contract no. DE-AC02-06CH11357). Use of the Stanford Synchrotron Radiation Lightsource at SLAC National Accelerator Laboratory is supported by the US DOE, Office of Science, Office of Basic Energy Sciences (contract no. DE-AC02-76SF00515). We extend our special thanks to G. S. Shekhawat, H. Choi and L. J. Lauhon (Northwestern) for the attempt of in situ atomic force microscopy and related discussions. J.S. and Q.Z. acknowledge expert technical assistance of R. Ziegler (Argonne) and thank E. Dufrense (Argonne) and M. Sutton (Mcgill) for insightful and fruitful discussion.

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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abstract = "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. 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{\textquoteright}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.",

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AU - Strzalka, Joseph

AU - Narayanan, Suresh

AU - Zhang, Qingteng

AU - Paulsen, Bryan D.

AU - Rivnay, Jonathan

AU - Takacs, Christopher J.

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AB - 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. 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.

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

Abstract

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