The Role of Side Chains and Hydration on Mixed Charge Transport in n ‐Type Polymer Films

Jokūbas Surgailis; Lucas Q. Flagg; Lee J. Richter; Victor Druet; Sophie Griggs; Xiaocui Wu; Stefania Moro; David Ohayon; Christina J. Kousseff; Adam Marks; Iuliana P. Maria; Hu Chen; Maximilian Moser; Giovanni Costantini; Iain McCulloch; Sahika Inal

doi:10.1002/adma.202313121

The Role of Side Chains and Hydration on Mixed Charge Transport in n ‐Type Polymer Films

Jokūbas Surgailis, Lucas Q. Flagg, Lee J. Richter, Victor Druet, Sophie Griggs, Xiaocui Wu, Stefania Moro, David Ohayon, Christina J. Kousseff, Adam Marks, Iuliana P. Maria, Hu Chen, Maximilian Moser, Giovanni Costantini, Iain McCulloch, Sahika Inal^*

^*Corresponding author for this work

Chemistry

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Abstract

Introducing ethylene glycol (EG) side chains to a conjugated polymer backbone is a well‐established synthetic strategy for designing organic mixed ion‐electron conductors (OMIECs). However, the impact that film swelling has on mixed conduction properties has yet to be scoped, particularly for electron‐transporting (n‐type) OMIECs. Here, the authors investigate the effect of the length of branched EG chains on mixed charge transport of n‐type OMIECs based on a naphthalene‐1,4,5,8‐tetracarboxylic‐diimide‐bithiophene backbone. Atomic force microscopy (AFM), grazing‐incidence wide‐angle X‐ray scattering (GIWAXS), and scanning tunneling microscopy (STM) are used to establish the similarities between the common‐backbone films in dry conditions. Electrochemical quartz crystal microbalance with dissipation monitoring (EQCM‐D) and in situ GIWAXS measurements reveal stark changes in film swelling properties and microstructure during electrochemical doping, depending on the side chain length. It is found that even in the loss of the crystallite content upon contact with the aqueous electrolyte, the films can effectively transport charges and that it is rather the high water content that harms the electronic interconnectivity within the OMIEC films. These results highlight the importance of controlling water uptake in the films to impede charge transport in n‐type electrochemical devices.

Original language	English
Article number	2313121
Journal	Advanced Materials
Early online date	30 Mar 2024
DOIs	https://doi.org/10.1002/adma.202313121
Publication status	E-pub ahead of print - 30 Mar 2024

Bibliographical note

Acknowledgments:
X.W. acknowledges co-funding from the European Union's Horizon 2020 research and innovation Marie Skłodowska-Curie Actions, under grant agreement no. 945380. S.M. acknowledges funding through an EU Chancellor's Scholarship by the University of Warwick. This publication is based upon work supported by King Abdullah University of Science and Technology (KAUST) Research Funding (KRF) under Award No. ORA-2021-CRG10-4650. G.C. and S.M. acknowledge support from a UK - Saudi Challenge Fund grant from the British Council's Going Global Partnerships programme. This research used beamline 11-BM (CMS) of the National Synchrotron Light Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. J.S. thanks Yizhou Zhong and Wentao Shan for providing devices for OECT characterization.

Open access publishing facilitated by King Abdullah University of Science and Technology, as part of the Wiley – King Abdullah University of Science and Technology (KAUST) agreement.

Keywords

swelling
in operando
quartz crystal microbalance
electrochemical transistors
organic mixed conductors

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Surgailis, J., Flagg, L. Q., Richter, L. J., Druet, V., Griggs, S., Wu, X., Moro, S., Ohayon, D., Kousseff, C. J., Marks, A., Maria, I. P., Chen, H., Moser, M., Costantini, G., McCulloch, I., & Inal, S. (2024). The Role of Side Chains and Hydration on Mixed Charge Transport in n ‐Type Polymer Films. Advanced Materials, Article 2313121. Advance online publication. https://doi.org/10.1002/adma.202313121

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title = "The Role of Side Chains and Hydration on Mixed Charge Transport in n ‐Type Polymer Films",

abstract = "Introducing ethylene glycol (EG) side chains to a conjugated polymer backbone is a well‐established synthetic strategy for designing organic mixed ion‐electron conductors (OMIECs). However, the impact that film swelling has on mixed conduction properties has yet to be scoped, particularly for electron‐transporting (n‐type) OMIECs. Here, the authors investigate the effect of the length of branched EG chains on mixed charge transport of n‐type OMIECs based on a naphthalene‐1,4,5,8‐tetracarboxylic‐diimide‐bithiophene backbone. Atomic force microscopy (AFM), grazing‐incidence wide‐angle X‐ray scattering (GIWAXS), and scanning tunneling microscopy (STM) are used to establish the similarities between the common‐backbone films in dry conditions. Electrochemical quartz crystal microbalance with dissipation monitoring (EQCM‐D) and in situ GIWAXS measurements reveal stark changes in film swelling properties and microstructure during electrochemical doping, depending on the side chain length. It is found that even in the loss of the crystallite content upon contact with the aqueous electrolyte, the films can effectively transport charges and that it is rather the high water content that harms the electronic interconnectivity within the OMIEC films. These results highlight the importance of controlling water uptake in the films to impede charge transport in n‐type electrochemical devices.",

keywords = "swelling, in operando, quartz crystal microbalance, electrochemical transistors, organic mixed conductors",

author = "Jokūbas Surgailis and Flagg, {Lucas Q.} and Richter, {Lee J.} and Victor Druet and Sophie Griggs and Xiaocui Wu and Stefania Moro and David Ohayon and Kousseff, {Christina J.} and Adam Marks and Maria, {Iuliana P.} and Hu Chen and Maximilian Moser and Giovanni Costantini and Iain McCulloch and Sahika Inal",

note = "Acknowledgments: X.W. acknowledges co-funding from the European Union's Horizon 2020 research and innovation Marie Sk{\l}odowska-Curie Actions, under grant agreement no. 945380. S.M. acknowledges funding through an EU Chancellor's Scholarship by the University of Warwick. This publication is based upon work supported by King Abdullah University of Science and Technology (KAUST) Research Funding (KRF) under Award No. ORA-2021-CRG10-4650. G.C. and S.M. acknowledge support from a UK - Saudi Challenge Fund grant from the British Council's Going Global Partnerships programme. This research used beamline 11-BM (CMS) of the National Synchrotron Light Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. J.S. thanks Yizhou Zhong and Wentao Shan for providing devices for OECT characterization. Open access publishing facilitated by King Abdullah University of Science and Technology, as part of the Wiley – King Abdullah University of Science and Technology (KAUST) agreement. ",

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doi = "10.1002/adma.202313121",

language = "English",

journal = "Advanced Materials",

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AU - Surgailis, Jokūbas

AU - Flagg, Lucas Q.

AU - Richter, Lee J.

AU - Druet, Victor

AU - Griggs, Sophie

AU - Wu, Xiaocui

AU - Moro, Stefania

AU - Ohayon, David

AU - Kousseff, Christina J.

AU - Marks, Adam

AU - Maria, Iuliana P.

AU - Chen, Hu

AU - Moser, Maximilian

AU - Costantini, Giovanni

AU - McCulloch, Iain

AU - Inal, Sahika

N1 - Acknowledgments: X.W. acknowledges co-funding from the European Union's Horizon 2020 research and innovation Marie Skłodowska-Curie Actions, under grant agreement no. 945380. S.M. acknowledges funding through an EU Chancellor's Scholarship by the University of Warwick. This publication is based upon work supported by King Abdullah University of Science and Technology (KAUST) Research Funding (KRF) under Award No. ORA-2021-CRG10-4650. G.C. and S.M. acknowledge support from a UK - Saudi Challenge Fund grant from the British Council's Going Global Partnerships programme. This research used beamline 11-BM (CMS) of the National Synchrotron Light Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. J.S. thanks Yizhou Zhong and Wentao Shan for providing devices for OECT characterization. Open access publishing facilitated by King Abdullah University of Science and Technology, as part of the Wiley – King Abdullah University of Science and Technology (KAUST) agreement.

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Y1 - 2024/3/30

N2 - Introducing ethylene glycol (EG) side chains to a conjugated polymer backbone is a well‐established synthetic strategy for designing organic mixed ion‐electron conductors (OMIECs). However, the impact that film swelling has on mixed conduction properties has yet to be scoped, particularly for electron‐transporting (n‐type) OMIECs. Here, the authors investigate the effect of the length of branched EG chains on mixed charge transport of n‐type OMIECs based on a naphthalene‐1,4,5,8‐tetracarboxylic‐diimide‐bithiophene backbone. Atomic force microscopy (AFM), grazing‐incidence wide‐angle X‐ray scattering (GIWAXS), and scanning tunneling microscopy (STM) are used to establish the similarities between the common‐backbone films in dry conditions. Electrochemical quartz crystal microbalance with dissipation monitoring (EQCM‐D) and in situ GIWAXS measurements reveal stark changes in film swelling properties and microstructure during electrochemical doping, depending on the side chain length. It is found that even in the loss of the crystallite content upon contact with the aqueous electrolyte, the films can effectively transport charges and that it is rather the high water content that harms the electronic interconnectivity within the OMIEC films. These results highlight the importance of controlling water uptake in the films to impede charge transport in n‐type electrochemical devices.

AB - Introducing ethylene glycol (EG) side chains to a conjugated polymer backbone is a well‐established synthetic strategy for designing organic mixed ion‐electron conductors (OMIECs). However, the impact that film swelling has on mixed conduction properties has yet to be scoped, particularly for electron‐transporting (n‐type) OMIECs. Here, the authors investigate the effect of the length of branched EG chains on mixed charge transport of n‐type OMIECs based on a naphthalene‐1,4,5,8‐tetracarboxylic‐diimide‐bithiophene backbone. Atomic force microscopy (AFM), grazing‐incidence wide‐angle X‐ray scattering (GIWAXS), and scanning tunneling microscopy (STM) are used to establish the similarities between the common‐backbone films in dry conditions. Electrochemical quartz crystal microbalance with dissipation monitoring (EQCM‐D) and in situ GIWAXS measurements reveal stark changes in film swelling properties and microstructure during electrochemical doping, depending on the side chain length. It is found that even in the loss of the crystallite content upon contact with the aqueous electrolyte, the films can effectively transport charges and that it is rather the high water content that harms the electronic interconnectivity within the OMIEC films. These results highlight the importance of controlling water uptake in the films to impede charge transport in n‐type electrochemical devices.

KW - swelling

KW - in operando

KW - quartz crystal microbalance

KW - electrochemical transistors

KW - organic mixed conductors

U2 - 10.1002/adma.202313121

DO - 10.1002/adma.202313121

M3 - Article

SN - 0935-9648

JO - Advanced Materials

JF - Advanced Materials

M1 - 2313121

ER -

The Role of Side Chains and Hydration on Mixed Charge Transport in n ‐Type Polymer Films

Abstract

Bibliographical note

Keywords

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