Transition metal-catalysed molecular n-doping of organic semiconductors

Han Guo; Chi Yuan Yang; Xianhe Zhang; Alessandro Motta; Kui Feng; Yu Xia; Yongqiang Shi; Ziang Wu; Kun Yang; Jianhua Chen; Qiaogan Liao; Yumin Tang; Huiliang Sun; Han Young Woo; Simone Fabiano; Antonio Facchetti; Xugang Guo

doi:10.1038/s41586-021-03942-0

Transition metal-catalysed molecular n-doping of organic semiconductors

Han Guo, Chi Yuan Yang, Xianhe Zhang, Alessandro Motta, Kui Feng, Yu Xia, Yongqiang Shi, Ziang Wu, Kun Yang, Jianhua Chen, Qiaogan Liao, Yumin Tang, Huiliang Sun, Han Young Woo, Simone Fabiano, Antonio Facchetti^*, Xugang Guo^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

208 Scopus citations

Abstract

Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices^1–9. N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (η) of less than 10%^1,10. An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability^1,5,6,9,11, which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd₂(dba)₃) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased η in a much shorter doping time and high electrical conductivities (above 100 S cm⁻¹; ref. ¹²). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications^{12, 13}.

Original language	English (US)
Pages (from-to)	67-73
Number of pages	7
Journal	Nature
Volume	599
Issue number	7883
DOIs	https://doi.org/10.1038/s41586-021-03942-0
State	Published - Nov 4 2021

Funding

Acknowledgements H.G. and X.G. gratefully acknowledge financial support from the National Natural Science Foundation of China (51903117 and 21774055) and the Shenzhen Science and Technology Innovation Commission (JCYJ20180504165709042). A.F. acknowledges AFOSR grant FA9550-18-1-0320. S.F. and C.-Y.Y. acknowledge financial support from the Swedish Research Council (2020-03243), Olle Engkvists Stiftelse (204-0256), VINNOVA (2020-05223),Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971), and the European Commission through the Marie Sklodowska-Curie project HORATES (GA-955837). A.M. acknowledges CINECA award no. HP10CC5WSY 2020 under the ISCRA initiative for computational resources. H.Y.W. acknowledges financial support from the National Research Foundation (NRF) of Korea (NRF-2019R1A2C2085290). We also acknowledge technical support from SUSTech Core Research Facilities. We thank H. Li, L. Lin, Z.-Y. Ren and Y.-H. Yang for performing ESI-MS and ESR measurements. We thank L. Safaric, Q. Li and Y. Liu (Linköping University) for assistance with GC, absorption and NMR measurements.

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title = "Transition metal-catalysed molecular n-doping of organic semiconductors",

abstract = "Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices1–9. N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (η) of less than 10%1,10. An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability1,5,6,9,11, which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd2(dba)3) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased η in a much shorter doping time and high electrical conductivities (above 100 S cm−1; ref. 12). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications12, 13.",

author = "Han Guo and Yang, {Chi Yuan} and Xianhe Zhang and Alessandro Motta and Kui Feng and Yu Xia and Yongqiang Shi and Ziang Wu and Kun Yang and Jianhua Chen and Qiaogan Liao and Yumin Tang and Huiliang Sun and Woo, {Han Young} and Simone Fabiano and Antonio Facchetti and Xugang Guo",

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AU - Liao, Qiaogan

AU - Tang, Yumin

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AB - Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices1–9. N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (η) of less than 10%1,10. An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability1,5,6,9,11, which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd2(dba)3) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased η in a much shorter doping time and high electrical conductivities (above 100 S cm−1; ref. 12). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications12, 13.

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Transition metal-catalysed molecular n-doping of organic semiconductors

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