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Kiefer, David; Kroon, Renee; Hofmann, Anna I; Sun, Hengda; Liu, Xianjie; Giovannitti, Alexander; Stegerer, Dominik; Cano, Alexander; Hynynen, Jonna; Yu, Liyang; Zhang, Yadong; Nai, Dingqi; Harrelson, Thomas F; Sommer, Michael; Moulé, Adam J; Kemerink, Martijn; Marder, Seth R; McCulloch, Iain; Fahlman, Mats; Fabiano, Simone; Müller, Christian
Nature materials, 02/2019, Letnik: 18, Številka: 2Journal Article
Molecular doping is a crucial tool for controlling the charge-carrier concentration in organic semiconductors. Each dopant molecule is commonly thought to give rise to only one polaron, leading to a maximum of one donor:acceptor charge-transfer complex and hence an ionization efficiency of 100%. However, this theoretical limit is rarely achieved because of incomplete charge transfer and the presence of unreacted dopant. Here, we establish that common p-dopants can in fact accept two electrons per molecule from conjugated polymers with a low ionization energy. Each dopant molecule participates in two charge-transfer events, leading to the formation of dopant dianions and an ionization efficiency of up to 200%. Furthermore, we show that the resulting integer charge-transfer complex can dissociate with an efficiency of up to 170%. The concept of double doping introduced here may allow the dopant fraction required to optimize charge conduction to be halved.
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