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Multivalent anions as universal latent electron donors

Author

Listed:
  • Cindy G. Tang

    (National University of Singapore)

  • Mazlan Nur Syafiqah

    (National University of Singapore)

  • Qi-Mian Koh

    (National University of Singapore)

  • Chao Zhao

    (National University of Singapore)

  • Jamal Zaini

    (National University of Singapore)

  • Qiu-Jing Seah

    (National University of Singapore)

  • Michael J. Cass

    (Cambridge Display Technology Limited)

  • Martin J. Humphries

    (Cambridge Display Technology Limited)

  • Ilaria Grizzi

    (Cambridge Display Technology Limited)

  • Jeremy H. Burroughes

    (Cambridge Display Technology Limited)

  • Rui-Qi Png

    (National University of Singapore)

  • Lay-Lay Chua

    (National University of Singapore
    National University of Singapore)

  • Peter K. H. Ho

    (National University of Singapore)

Abstract

Electrodes with low work functions are required to efficiently inject electrons into semiconductor devices. However, when the work function drops below about 4 electronvolts, the electrode suffers oxidation in air, which prevents its fabrication in ambient conditions. Here we show that multivalent anions such as oxalate, carbonate and sulfite can act as powerful latent electron donors when dispersed as small ion clusters in a matrix, while retaining their ability to be processed in solution in ambient conditions. The anions in these clusters can even n-dope the semiconductor core of π-conjugated polyelectrolytes that have low electron affinities, through a ground-state doping mechanism that is further amplified by a hole-sensitized or photosensitized mechanism in the device. A theoretical analysis of donor levels of these anions reveals that they are favourably upshifted from ionic lattices by a decrease in the Coulomb stabilization of small ion clusters, and by irreversibility effects. We attain an ultralow effective work function of 2.4 electronvolts with the polyfluorene core. We realize high-performance, solution-processed, white-light-emitting diodes and organic solar cells using polymer electron injection layers with these universal anion donors, demonstrating a general approach to chemically designed and ambient-processed Ohmic electron contacts for semiconductor devices.

Suggested Citation

  • Cindy G. Tang & Mazlan Nur Syafiqah & Qi-Mian Koh & Chao Zhao & Jamal Zaini & Qiu-Jing Seah & Michael J. Cass & Martin J. Humphries & Ilaria Grizzi & Jeremy H. Burroughes & Rui-Qi Png & Lay-Lay Chua &, 2019. "Multivalent anions as universal latent electron donors," Nature, Nature, vol. 573(7775), pages 519-525, September.
  • Handle: RePEc:nat:nature:v:573:y:2019:i:7775:d:10.1038_s41586-019-1575-7
    DOI: 10.1038/s41586-019-1575-7
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    Citations

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    Cited by:

    1. Zhao-Siu Tan & Zaini Jamal & Desmond W. Y. Teo & Hor-Cheng Ko & Zong-Long Seah & Hao-Yu Phua & Peter K. H. Ho & Rui-Qi Png & Lay-Lay Chua, 2024. "Optimization of fluorinated phenyl azides as universal photocrosslinkers for semiconducting polymers," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    2. Cindy Guanyu Tang & Mazlan Nur Syafiqah & Qi-Mian Koh & Mervin Chun-Yi Ang & Kim-Kian Choo & Ming-Ming Sun & Martin Callsen & Yuan-Ping Feng & Lay-Lay Chua & Rui-Qi Png & Peter K. H. Ho, 2023. "Water binding and hygroscopicity in π-conjugated polyelectrolytes," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    3. Xiao Tan & Dehai Dou & Lay-Lay Chua & Rui-Qi Png & Daniel G. Congrave & Hugo Bronstein & Martin Baumgarten & Yungui Li & Paul W. M. Blom & Gert-Jan A. H. Wetzelaer, 2024. "Inverted device architecture for high efficiency single-layer organic light-emitting diodes with imbalanced charge transport," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    4. Weeratunge, Hansani & Aditya, Gregorius Riyan & Dunstall, Simon & de Hoog, Julian & Narsilio, Guillermo & Halgamuge, Saman, 2021. "Feasibility and performance analysis of hybrid ground source heat pump systems in fourteen cities," Energy, Elsevier, vol. 234(C).
    5. Sugawara, Carmen Luca & Kim, Hea-Won & Modić Stanke, Koraljka & Krasniqi, Vjollca & Basic, Sanela, 2023. "The role of community-university engagement in strengthening local community capacity in Southeastern Europe," International Journal of Educational Development, Elsevier, vol. 98(C).
    6. Ziyang Liu & Xiao Li & Yang Lu & Chen Zhang & Yuewei Zhang & Tianyu Huang & Dongdong Zhang & Lian Duan, 2022. "In situ-formed tetrahedrally coordinated double-helical metal complexes for improved coordination-activated n-doping," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    7. Bo Tong & Jinhong Du & Lichang Yin & Dingdong Zhang & Weimin Zhang & Yu Liu & Yuning Wei & Chi Liu & Yan Liang & Dong-Ming Sun & Lai-Peng Ma & Hui-Ming Cheng & Wencai Ren, 2022. "A polymer electrolyte design enables ultralow-work-function electrode for high-performance optoelectronics," Nature Communications, Nature, vol. 13(1), pages 1-12, December.

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