A Polymer Physics Approach to Organic Mixed Conductors

Loren G. Kaake^a

^aSimon Fraser University, Chemistry, 8888 University Drive, Burnaby, 0, Canada

Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#OMIEC - Understanding Mixed Ionic-Electronic Conductors

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Natalie Banerji and Olivier Bardagot

Invited Speaker, Loren G. Kaake, presentation 131
Publication date: 28th August 2024

Organic mixed conductors have the ability to transport both ions and electronic charge carriers. Many devices which leverage this property have been developed, including biosensors,[1] energy storage materials,[2] light emitting electrochemical cells,[3] organic electrochemical transistors,[4] and neuromorphic computing elements,[5] to name a few. In addition, the problem is connected to the earliest days of organic electronics research through measurements via standard electrochemical methods.[6] More broadly, the problem of mixed conduction sits at the crossroads of polymer physics and activity-based approaches to electrolyte equilibria. I will present results that demonstrate the fundamental mechanisms operating in organic electrochemical transistors,[7] along with key structure-property relationships that govern ion dynamics.[8] Approaching the problem from a polymer thermodynamics perspective also provides insight into thin film swelling behavior[9] and interfacial stability.[10] The perspective treats doped polymer films as solid state solutions, describing local field interactions as the correct first order effect. Of course, pi-conjugated polymers are not uniform homogeneous materials, and modifications to the perspective that take polymer morphology into account will be discussed. Lastly, we will present results that compare organic electrochemical materials with activated carbon and demonstrate that they do not resemble each other in any meaningful way beyond lumped circuit element models.

References:

[1] Bernards, D. A.; Macaya, D. J.; Nikolou, M.; DeFranco, J. A.; Takamatsu, S.; Malliaras, G. G., Enzymatic sensing with organic electrochemical transistors. J. Mater. Chem. 2008, 18 (1), 116-120.

[2] Milczarek, G.; Inganas, O., Renewable Cathode Materials from Biopolymer/Conjugated Polymer Interpenetrating Networks. Science 2012, 335 (6075), 1468-1471.

[3] Shao, Y.; Bazan, G. C.; Heeger, A. J., Long-lifetime polymer light-emitting electrochemical cells. Adv. Mater. 2007, 19 (3), 365-370.

[4] Chao, S.; Wrighton, M. S., Solid-State Microelectrochemistry - Electrical Characteristics of a Solid-State Microelectrochemical Transistor Based on Poly(3-Methylthiophene). J. Am. Chem. Soc. 1987, 109 (7), 2197-2199.

[5] Fuller, E. J.; Keene, S. T.; Melianas, A.; Wang, Z. R.; Agarwal, S.; Li, Y. Y.; Tuchman, Y.; James, C. D.; Marinella, M. J.; Yang, J. J.; Salleo, A.; Talin, A. A., Parallel programming of an ionic floating-gate memory array for scalable neuromorphic computing. Science 2019, 364 (6440), 570-574.

[6] Diaz, A. F.; Logan, J. A., Electroactive Polyaniline Films. J. Electroanal. Chem. 1980, 111 (1), 111-114.

[7] Shiri, P.; Neusser, D.; Malacrida, C.; Ludwigs, S.; Kaake, L. G., Mixed Ion-Carrier Diffusion in Poly(3-hexyl thiophene)/Perchlorate Electrochemical Systems. The Journal of Physical Chemistry C 2021, 125 (1), 536-545.

[8] Shiri, P.; Dacanay, E. J. S.; Hagen, B.; Kaake, L. G., Vogel–Tammann–Fulcher model for charging dynamics in an organic electrochemical transistor. J. Mater. Chem. C 2019, 7, 12935-12941.

[9] Kaake, L. G.; Gompf, B.; Ludwigs, S., Electrochemical and Solvent-Driven Swelling in a Conducting Polymer Film. Chem. Mater. 2023, 35 (11), 4532-4540.

[10] Kaake, L. G.; Paulsen, B. D.; Frisbie, C. D.; Zhu, X. Y., Mixing at the charged interface of a polymer semiconductor and a polyelectrolyte dielectric. J. Phys. Chem. Lett. 2010, 1 (5), 862-867.

Acknowledgements:

L.G.K. acknowledges funding from the Natural Sciences and Engineering Research Council of Canada (NSERC) through the Discovery Grants Program (RGPIN-2015-05981 and RGPIN-2022-03525). L.G.K also acknowledges funding through NSERC Green Electronics Network (GreEN) (NETGP 508526-17).

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