Understanding asymmetric switching times in accumulation mode organic electrochemical transistors
Source abstract
Abstract
Understanding the factors underpinning device switching times is crucial for the implementation of organic electrochemical transistors in neuromorphic computing, bioelectronics and real-time sensing applications. Existing models of device operation cannot explain the experimental observations that turn-off times are generally much faster than turn-on times in accumulation mode organic electrochemical transistors. Here, using operando optical microscopy, we image the local doping level of the transistor channel and show that turn-on occurs in two stages-propagation of a doping front, followed by uniform doping-while turn-off occurs in one stage. We attribute the faster turn-off to a combination of engineering as well as physical and chemical factors including channel geometry, differences in doping and dedoping kinetics and the phenomena of carrier-density-dependent mobility. We show that ion transport limits the operation speed in our devices. Our study provides insights into the kinetics of organic electrochemical transistors and guidelines for engineering faster organic electrochemical transistors.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Conducting polymers and applications · Advanced Memory and Neural Computing · Organic Electronics and Photovoltaics
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References (56)
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1. Guo, K. et al. Rapid single-molecule detection of COVID-19 and MERS antigens via nanobody-functionalized organic electrochemical transistors. Nat. Biomed. Eng. 5, 666–677 (2021).10.1038/s41551-021-00734-9 ↗
2. Bischak, C. G., Flagg, L. Q. & Ginger, D. S. Ion exchange gels allow organic electrochemical transistor operation with hydrophobic polymers in aqueous solution. Adv. Mater. 32, 2002610 (2020).10.1002/adma.202002610 ↗
3. Strakosas, X., Bongo, M. & Owens, R. M. The organic electrochemical transistor for biological applications. J. Appl. Polym. Sci. 132, 41735 (2015).10.1002/app.41735 ↗
4. Pappa, A. M. et al. Organic transistor arrays integrated with finger-powered microfluidics for multianalyte saliva testing. Adv. Healthc. Mater. 5, 2295–2302 (2016).10.1002/adhm.201600494 ↗
5. Huang, W. et al. Vertical organic electrochemical transistors for complementary circuits. Nature 613, 496–502 (2023).10.1038/s41586-022-05592-2 ↗
6. Andersson Ersman, P. et al. All-printed large-scale integrated circuits based on organic electrochemical transistors. Nat. Commun. 10, 5053 (2019).10.1038/s41467-019-13079-4 ↗
7. Fuller, E. J. et al. Parallel programming of an ionic floating-gate memory array for scalable neuromorphic computing. Science 364, 570–574 (2019).10.1126/science.aaw5581 ↗
8. Harikesh, P. C. et al. Ion-tunable antiambipolarity in mixed ion–electron conducting polymers enables biorealistic organic electrochemical neurons. Nat. Mater. 22, 242–248 (2023).10.1038/s41563-022-01450-8 ↗
9. Chen, S. E., Giridharagopal, R. & Ginger, D. S. Artificial neuron transmits chemical signals. Nat. Mater. 22, 416–418 (2023).10.1038/s41563-023-01509-0 ↗
10. Sarkar, T. et al. An organic artificial spiking neuron for in situ neuromorphic sensing and biointerfacing. Nat. Electron. 5, 774–783 (2022).10.1038/s41928-022-00859-y ↗
11. Yamamoto, S. & Malliaras, G. G. Controlling the neuromorphic behavior of organic electrochemical transistors by blending mixed and ion conductors. ACS Appl. Electron. Mater. 2, 2224–2228 (2020).10.1021/acsaelm.0c00203 ↗
12. Gkoupidenis, P., Schaefer, N., Garlan, B. & Malliaras, G. G. Neuromorphic functions in PEDOT:PSS organic electrochemical transistors. Adv. Mater. 27, 7176–7180 (2015).10.1002/adma.201503674 ↗
13. Khodagholy, D. et al. High transconductance organic electrochemical transistors. Nat. Commun. 4, 2133 (2013).10.1038/ncomms3133 ↗
14. Lin, P., Yan, F. & Chan, H. L. W. Ion-sensitive properties of organic electrochemical transistors. Appl. Mater. Interfaces 2, 1637–1641 (2010).10.1021/am100154e ↗
15. Ghittorelli, M. et al. High-sensitivity ion detection at low voltages with current-driven organic electrochemical transistors. Nat. Commun. 9, 1441 (2018).10.1038/s41467-018-03932-3 ↗
16. Gualandi, I. et al. Selective detection of dopamine with an all PEDOT:PSS organic electrochemical transistor. Sci. Rep. 6, 35419 (2016).10.1038/srep35419 ↗
17. Xie, K. et al. Organic electrochemical transistor arrays for real-time mapping of evoked neurotransmitter release in vivo. eLife 9, e50345 (2020).10.7554/eLife.50345 ↗
18. Khodagholy, D. et al. In vivo recordings of brain activity using organic transistors. Nat. Commun. 4, 1575 (2013).10.1038/ncomms2573 ↗
19. Tang, X., Shen, H., Zhao, S., Li, N. & Liu, J. Flexible brain–computer interfaces. Nat. Electron. 6, 109–118 (2023).10.1038/s41928-022-00913-9 ↗
20. Berggren, M., Głowacki, E. D., Simon, D. T., Stavrinidou, E. & Tybrandt, K. In vivo organic bioelectronics for neuromodulation. Chem. Rev. 122, 4826–4846 (2022).10.1021/acs.chemrev.1c00390 ↗
21. Go, G.-T., Lee, Y., Seo, D.-G. & Lee, T.-W. Organic neuroelectronics: from neural interfaces to neuroprosthetics. Adv. Mater. 34, 2201864 (2022).10.1002/adma.202201864 ↗
22. Van DeBurgt, Y., Melianas, A., Keene, S. T., Malliaras, G. & Salleo, A. Organic electronics for neuromorphic computing. Nat. Electron. 1, 386–397 (2018).10.1038/s41928-018-0103-3 ↗
23. Gumyusenge, A., Melianas, A., Keene, S. T. & Salleo, A. Materials strategies for organic neuromorphic devices. Annu. Rev. Mater. Res. 51, 47–71 (2021).10.1146/annurev-matsci-080619-111402 ↗
24. Rivnay, J. et al. Organic electrochemical transistors. Nat. Rev. Mater. 3, 17086 (2018).10.1038/natrevmats.2017.86 ↗
25. Zeglio, E. & Inganäs, O. Active materials for organic electrochemical transistors. Adv. Mater. 30, 1800941 (2018).10.1002/adma.201800941 ↗
26. Kukhta, N. A., Marks, A. & Luscombe, C. K. Molecular design strategies toward improvement of charge injection and ionic conduction in organic mixed ionic–electronic conductors for organic electrochemical transistors. Chem. Rev. 122, 4325–4355 (2022).10.1021/acs.chemrev.1c00266 ↗
27. He, Y., Kukhta, N. A., Marks, A. & Luscombe, C. K. The effect of side chain engineering on conjugated polymers in organic electrochemical transistors for bioelectronic applications. J. Mater. Chem. C 10, 2314–2332 (2022).10.1039/D1TC05229B ↗
28. Paulsen, B. D., Tybrandt, K., Stavrinidou, E. & Rivnay, J. Organic mixed ionic–electronic conductors. Nat. Mater. 19, 13–26 (2020).10.1038/s41563-019-0435-z ↗
29. Flagg, L. Q. et al. P-Type electrochemical doping can occur by cation expulsion in a high-performing polymer for organic electrochemical transistors. ACS Mater. Lett. 2, 254–260 (2020).10.1021/acsmaterialslett.9b00501 ↗
30. Bernards, D. A. & Malliaras, G. G. Steady-state and transient behavior of organic electrochemical transistors. Adv. Funct. Mater. 17, 3538–3544 (2007).10.1002/adfm.200601239 ↗
31. Ohayon, D., Druet, V. & Inal, S. A guide for the characterization of organic electrochemical transistors and channel materials. Chem. Soc. Rev. 52, 1001–1023 (2023).10.1039/D2CS00920J ↗
32. Inal, S., Malliaras, G. G. & Rivnay, J. Benchmarking organic mixed conductors for transistors. Nat. Commun. 8, 1767 (2017).10.1038/s41467-017-01812-w ↗
33. Li, P. & Lei, T. Molecular design strategies for high-performance organic electrochemical transistors. J. Polym. Sci. 60, 377–392 (2022).10.1002/pol.20210503 ↗
34. Gentile, F. et al. A theoretical model for the time varying current in organic electrochemical transistors in a dynamic regime. Org. Electron. 35, 59–64 (2016).10.1016/j.orgel.2016.05.001 ↗
35. Faria, G. C., Duong, D. T. & Salleo, A. On the transient response of organic electrochemical transistors. Org. Electron. 45, 215–221 (2017).10.1016/j.orgel.2017.03.021 ↗
36. Paudel, P. R. et al. The transient response of organic electrochemical transistors. Adv. Theory Simul. 5, 2100563 (2022).10.1002/adts.202100563 ↗
37. Keene, S. T. et al. Hole-limited electrochemical doping in conjugated polymers. Nat. Mater. 22, 1121–1127 (2023).10.1038/s41563-023-01601-5 ↗
38. Ersman, P. A. et al. Screen printed digital circuits based on vertical organic electrochemical transistors. Flex. Print. Electron. 2, 045008 (2017).10.1088/2058-8585/aa903a ↗
39. Butler, J. A. V. Studies in heterogeneous equilibria. Part II.—The kinetic interpretation of the nernst theory of electromotive force. Trans. Faraday Soc. 19, 729–733 (1924).10.1039/TF9241900729 ↗
40. Butler, J. A. V. Studies in heterogeneous equilibria. Part III. A kinetic theory of reversible oxidation potentials at inert electrodes. Trans. Faraday Soc. 19, 734–739 (1924).10.1039/tf9241900734 ↗
41. Erdey-Grúz, T. & Volmer, M. Zur theorie der wasserstoff überspannung. Z. Phys. Chem. 150A, 203–213 (1930).10.1515/zpch-1930-15020 ↗
42. Bischak, C. G. et al. A reversible structural phase transition by electrochemically-driven ion injection into a conjugated polymer. J. Am. Chem. Soc. 142, 7434–7442 (2020).10.1021/jacs.9b12769 ↗
43. Flagg, L. Q. et al. Polymer crystallinity controls water uptake in glycol side-chain polymer organic electrochemical transistors. J. Am. Chem. Soc. 141, 4345–4354 (2019).10.1021/jacs.8b12640 ↗
44. Chen, S. E. et al. Impact of varying side chain structure on organic electrochemical transistor performance: a series of oligoethylene glycol-substituted polythiophenes. J. Mater. Chem. A 10, 10738–10749 (2022).10.1039/D2TA00683A ↗
45. Neusser, D. et al. High conductivities of disordered P3HT films by an electrochemical doping strategy. Chem. Mater. 32, 6003–6013 (2020).10.1021/acs.chemmater.0c01293 ↗
46. Hornberger, L. S., Neusser, D., Malacrida, C., Kaake, L. G. & Ludwigs, S. How charge trapping affects the conductivity of electrochemically doped poly(3-hexylthiophene) films. Appl. Phys. Lett. 119, 163301 (2021).10.1063/5.0056484 ↗
47. Jackson, S. R., Kingsford, R. L., Collins, G. W. & Bischak, C. G. Crystallinity determines ion injection kinetics and local ion density in organic mixed conductors. Chem. Mater. 35, 5392–5400 (2023).10.1021/acs.chemmater.3c00657 ↗
48. Friedlein, J. T., Shaheen, S. E., Malliaras, G. G. & McLeod, R. R. Optical measurements revealing nonuniform hole mobility in organic electrochemical transistors. Adv. Electron. Mater. 1, 1500189 (2015).10.1002/aelm.201500189 ↗
49. Tanase, C., Meijer, E. J., Blom, P. W. M. & DeLeeuw, D. M. Unification of the hole transport in polymeric field-effect transistors and light-emitting diodes. Phys. Rev. Lett. 9, 216601 (2003).10.1103/PhysRevLett.91.216601 ↗
50. Bässler, H., Kroh, D., Schauer, F., Nádaždy, V. & Köhler, A. Mapping the density of states distribution of organic semiconductors by employing energy resolved–electrochemical impedance spectroscopy. Adv. Funct. Mater. 31, 2007738 (2021).10.1002/adfm.202007738 ↗
51. Flagg, L. Q., Giridharagopal, R., Guo, J. & Ginger, D. S. Anion-dependent doping and charge transport in organic electrochemical transistors. Chem. Mater. 30, 5380–5389 (2018).10.1021/acs.chemmater.8b02220 ↗
52. Wu, R., Paulsen, B. D., Ma, Q. & Rivnay, J. Mass and charge transport kinetics in an organic mixed ionic–electronic conductor. Chem. Mater. 34, 9699–9710 (2022).10.1021/acs.chemmater.2c02476 ↗
53. Colucci, R., Barbosa, H. F. D. P., Günther, F., Cavassin, P. & Faria, G. C. Recent advances in modeling organic electrochemical transistors. Flex. Print. Electron. 5, 013001 (2020).10.1088/2058-8585/ab601b ↗
54. Guo, J. et al. Hydration of a side-chain-free n-type semiconducting ladder polymer driven by electrochemical doping. J. Am. Chem. Soc. 145, 1866–1876 (2023).10.1021/jacs.2c11468 ↗
55. West, S. M. et al. Phenazine-substituted poly(benzimidazobenzophenanthrolinedione): electronic structure, thin film morphology, electron transport, and mechanical properties of an n-type semiconducting ladder polymer. Macromolecules 56, 2081–2091 (2023).10.1021/acs.macromol.2c01999 ↗
56. Zhang, Z. et al. Modulate molecular interaction between hole extraction polymers and lead ions toward hysteresis-free and efficient perovskite solar cells. Adv. Mater. Interfaces 5, 1800090 (2018).10.1002/admi.201800090 ↗