Overcoming the water oxidative limit for ultra-high-workfunction hole-doped polymers

Qi-Mian Koh, Cindy Guanyu Tang, Mervin Chun-Yi Ang, Kim-Kian Choo, Qiu-Jing Seah, Rui-Qi Png (), Lay-Lay Chua () and Peter K. H. Ho
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Qi-Mian Koh: National University of Singapore
Cindy Guanyu Tang: National University of Singapore
Mervin Chun-Yi Ang: National University of Singapore
Kim-Kian Choo: National University of Singapore
Qiu-Jing Seah: National University of Singapore
Rui-Qi Png: National University of Singapore
Lay-Lay Chua: National University of Singapore
Peter K. H. Ho: National University of Singapore

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract It is widely thought that the water-oxidation reaction limits the maximum work function to about 5.25 eV for hole-doped semiconductors exposed to the ambient, constrained by the oxidation potential of air-saturated water. Here, we show that polymer organic semiconductors, when hole-doped, can show work functions up to 5.9 eV, and yet remain stable in the ambient. We further show that de-doping of the polymer is not determined by the oxidation of bulk water, as previously thought, due to its general absence, but by the counter-balancing anion and its ubiquitously hydrated complexes. The effective donor levels of these species, representing the edge of the ‘chemical’ density of states, can be depressed to about 6.0 eV below vacuum level. This can be achieved by raising the oxidation potential for hydronium generation, using large super-acid anions that are themselves also stable against oxidation. In this way, we demonstrate that poly(fluorene-alt-triarylamine) derivatives with tethered perfluoroalkyl-sulfonylimidosulfonyl anions can provide ambient solution-processability directly in the ultrahigh-workfunction hole-doped state to give films with good thermal stability. These results lay the path for design of soft materials for battery, bio-electronic and thermoelectric applications.

Date: 2021
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DOI: 10.1038/s41467-021-23347-x

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