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Solution-processed light-emitting electrochemical cells: challenges and opportunities
Umeå University, Faculty of Science and Technology, Department of Physics. (Organic and Photonic Electronics Group)ORCID iD: 0000-0002-8933-2049
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Our world is filling up with electronics. High-tech gadgets are integrated everywhere, from smart fridges able to track expiry dates and food usage, to microchip implants that let us unlock doors and pay with our hands. As innovative as they are, these new products and the many more to come impose new requirements on materials and fabrication methods. For instance, emerging electronic technologies that deliver light emission such as smart labels, authenticity features and light-based medical therapies, are often required to be flexible, see-through and low-cost, and in addition sustainable to fabricate, operate and recycle.

In response to these challenges, the light-emitting industry is turning to organic electronics for solutions, a field that promises resource-efficient fabrication using environmentally benign materials. An interesting proposal is that of the light-emitting electrochemical cell (LEC), which, thanks to its simple structure, is well suitedfor high-throughput fabrication. The LEC is in many aspects a smart device, able to reorganize itself during operation via the electrochemical action of mobile ions, which create the injection and transport layers that require additional fabrication steps in other technologies. This elegant behavior makes the LEC tolerant to a large array of materials and fabrication methods, and hence a good fit for many applications.

Yet the LEC is still today a scientific curiosity rather than an actual commercial solution and among the very few prototypes available on the market, none are able to meet the combined performance, resource efficiency and sustainability criteria. As a matter of fact, of the three layers that make an LEC, i.e., two electrodes surrounding an active material, only the later meet these requirements thanks to a strong recent research effort. In comparison, the electrodes have received little attention and are almost exclusively comprising metals or metal oxides deposited by time- and energy-expensive fabrication methods, making the LEC as a whole unfit for many applications.

In an effort to push the LEC toward the untapped commercial niche of low-cost lighting, we tackle the problem of electrode fabrication with resource-efficiency in mind. We first show that up-scalable spray coating of inks under ambient air is a viable mean of fabrication for both active materials and electrodes alike. However, in doing so, we find that we create electrode interfaces that are open to ion transfer; an up-to-now overlooked issue that needs careful consideration when designing solution-processed LECs. Building on our discovery, we demonstrate that it is possible to fabricate an LEC entirely by using spray coating metal-free and organic inks; thereby demonstrating that an all-organic, metal-free and resource-efficient LEC is possible.

I hope that our efforts will encourage others to work on solution-processed LECs, electrodes included, and develop ready-to-use products.

Place, publisher, year, edition, pages
Umeå: Umeå University , 2023. , p. 50
Keywords [en]
Light-emitting electrochemical cell, PEDOT:PSS, Photonics, Ion transfer, Solution-based fabrication
National Category
Other Physics Topics
Research subject
Electronics; Materials Science; Ion Physics
Identifiers
URN: urn:nbn:se:umu:diva-206243ISBN: 978-91-8070-027-6 (electronic)ISBN: 978-91-8070-026-9 (print)OAI: oai:DiVA.org:umu-206243DiVA, id: diva2:1747774
Public defence
2023-04-26, Hörsal NAT.D.410, Naturvetarhuset, Umeå, 09:30 (English)
Opponent
Supervisors
Available from: 2023-04-05 Created: 2023-03-31 Last updated: 2023-03-31Bibliographically approved
List of papers
1. Solution -based fabrication of the top electrode in light -emitting electrochemical cells
Open this publication in new window or tab >>Solution -based fabrication of the top electrode in light -emitting electrochemical cells
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2020 (English)In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 84, article id 105812Article in journal (Refereed) Published
Abstract [en]

The light-emitting electrochemical cell (LEC) has demonstrated capacity for cost- and material-efficient solution-based fabrication of the active material under ambient air. In this context, it is notable that corresponding reports on a scalable solution-based fabrication of the electrodes, particularly the top electrode, are rare. We address this issue through the demonstration of a transparent LEC, which is fabricated under ambient air by sequential spray deposition of a hydrophobic conjugated-polymer:ionic-liquid blend ink as the active material and a hydrophilic poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) ink as the transparent top electrode. Such an optimized LEC delivers a luminance of 360 cd/m2 at a power efficacy of 1.6 lm/W, which is on par with the performance of a corresponding LEC device equipped with a vacuum-deposited and reflective metal top electrode. This implies that the entire LEC device indeed can be fabricated with solution-based processes and deliver a good performance, which is critical if the LEC technology is going to fulfil its low-cost potential.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Solution-processed transparent electrode, Transparent light-emission device, Light-emitting electrochemical cellPEDOT, PSS
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:umu:diva-173299 (URN)10.1016/j.orgel.2020.105812 (DOI)000540714800015 ()2-s2.0-85085275396 (Scopus ID)
Funder
Swedish Research CouncilSwedish Energy AgencyCarl Tryggers foundation The Kempe FoundationsVästerbotten County CouncilBertil & Britt Svenssons Stiftelse för Belysningsteknik
Available from: 2020-07-06 Created: 2020-07-06 Last updated: 2023-03-31Bibliographically approved
2. Evidence and Effects of Ion Transfer at Active-Material/Electrode Interfaces in Solution-Fabricated Light-Emitting Electrochemical Cells
Open this publication in new window or tab >>Evidence and Effects of Ion Transfer at Active-Material/Electrode Interfaces in Solution-Fabricated Light-Emitting Electrochemical Cells
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2021 (English)In: Advanced Electronic Materials, E-ISSN 2199-160X, Vol. 7, no 8, article id 2100253Article in journal (Refereed) Published
Abstract [en]

The light-emitting electrochemical cell (LEC) allows for energy- and cost-efficient printing and coating fabrication of its entire device structure, including both electrodes and the single-layer active material. This attractive fabrication opportunity is enabled by the electrochemical action of mobile ions in the active material. However, a related and up to now overlooked issue is that such solution-fabricated LECs commonly comprise electrode/active-material interfaces that are open for transfer of the mobile ions, and it is herein demonstrated that a majority of the mobile anions in a common spray-coated active material can transfer into a spray-coated poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) positive electrode during LEC operation. Since it is well established that the mobile ion concentration in the active material has a profound influence on the LEC performance, this significant ion transfer is an important factor that should be considered in the design of low-cost LEC devices that deliver high performance.

Place, publisher, year, edition, pages
Wiley-Blackwell Publishing Inc., 2021
Keywords
active-material design, electrode electrochemistry, ion transfer, light-emitting electrochemical cell, PEDOT:PSS, solution fabrication
National Category
Materials Chemistry Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:umu:diva-185329 (URN)10.1002/aelm.202100253 (DOI)000662108100001 ()2-s2.0-85108074845 (Scopus ID)
Funder
Carl Tryggers foundation The Kempe FoundationsOlle Engkvists stiftelseInterreg NordBertil & Britt Svenssons Stiftelse för BelysningsteknikSwedish Research CouncilSwedish Energy AgencyRegion Västerbotten
Available from: 2021-06-28 Created: 2021-06-28 Last updated: 2023-03-31Bibliographically approved
3. Ion transfer into solution-processed electrodes can significantly shift the p-n junction and emission efficiency of light-emitting electrochemical cells
Open this publication in new window or tab >>Ion transfer into solution-processed electrodes can significantly shift the p-n junction and emission efficiency of light-emitting electrochemical cells
2022 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 121, no 23, article id 231102Article in journal (Refereed) Published
Abstract [en]

A light-emitting electrochemical cell (LEC) comprises mobile ions in its active material, which enable for in situ formation of a p-n junction by electrochemical doping. The position of this emissive p-n junction in the interelectrode gap is important, because it determines whether the emission is affected by constructive or destructive interference. An appealing LEC feature is that the entire device can be fabricated by low-cost solution-based printing and coating. Here, we show, somewhat unexpectedly, that the replacement of conventional vacuum-deposited indium-tin-oxide (ITO) for the positive anode with solution-processed poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) can result in an increase in the peak light-emission output by 75%. We demonstrate that this emission increase is due to that the p-n junction shifts from a position of destructive interference in the center of the interelectrode gap with ITO to a position of constructive interference closer to the anode with PEDOT:PSS. We rationalize the anodic p-n junction shift by significant anion transfer into the soft and porous PEDOT:PSS electrode during LEC operation, which is prohibited for the ITO electrode because of its compact and hard nature. Our study, thus, contributes with important design criteria for the attainment of efficient light emission from solution-processed LEC devices.

Place, publisher, year, edition, pages
American Institute of Physics (AIP), 2022
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:umu:diva-202064 (URN)10.1063/5.0123469 (DOI)000894763400004 ()2-s2.0-85144449170 (Scopus ID)
Available from: 2023-01-03 Created: 2023-01-03 Last updated: 2023-09-05Bibliographically approved
4. Metal-free and transparent light-emitting devices fabricated by sequentialspray coating
Open this publication in new window or tab >>Metal-free and transparent light-emitting devices fabricated by sequentialspray coating
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(English)Manuscript (preprint) (Other academic)
National Category
Other Physics Topics
Identifiers
urn:nbn:se:umu:diva-206245 (URN)
Available from: 2023-03-31 Created: 2023-03-31 Last updated: 2023-03-31

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Auroux, Etienne

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