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Abstract Organic doping is widely used for defining the majority charge carriers of organic thin films, tuning the Fermi level, and improving and stabilizing the performance of organic light‐emitting diodes and organic solar cells. However, in contrast to inorganic semiconductors, the doping concentrations commonly used are quite high (in the wt% range). Such high concentrations not only limit the scope of doping in organic field‐effect transistors (OFETs), but also limit the doping process itself resulting in a low doping efficiency. Here, the mechanism of doping at ultralow doping concentrations is studied. Doped C60metal‐oxide‐semiconductor (MOS) junctions are used to study doping at the 100 ppm level. With the help of a small‐signal drift‐diffusion model, it is possible to disentangle effects of traps at the gate dielectric/organic semiconductor interface from effects of doping and to determine the doping efficiency and activation energy of the doping process. Doped C60OFETs with an ultralow operation voltage of 800 mV and an excellent on/off ratio of up to 107are realized. The devices have low subthreshold swing in the range of 80 mV dec−1and a large transconductance of up to 8 mS mm−1.
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Abstract Chemical doping is an important approach to manipulating charge-carrier concentration and transport in organic semiconductors (OSCs)1–3and ultimately enhances device performance4–7. However, conventional doping strategies often rely on the use of highly reactive (strong) dopants8–10, which are consumed during the doping process. Achieving efficient doping with weak and/or widely accessible dopants under mild conditions remains a considerable challenge. Here, we report a previously undescribed concept for the photocatalytic doping of OSCs that uses air as a weak oxidant (p-dopant) and operates at room temperature. This is a general approach that can be applied to various OSCs and photocatalysts, yielding electrical conductivities that exceed 3,000 S cm–1. We also demonstrate the successful photocatalytic reduction (n-doping) and simultaneous p-doping and n-doping of OSCs in which the organic salt used to maintain charge neutrality is the only chemical consumed. Our photocatalytic doping method offers great potential for advancing OSC doping and developing next-generation organic electronic devices.
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While p-type BiCuSeO is a well-known mid-temperature oxide thermoelectric (TE) material, computations predict that superior TE performance can be realized through n-type doping. In this study, we use first-principles defect calculations to show that Cu vacancies are responsible for the native p-type self doping; yet, we find that BiCuSeO is n-type dopable under Cu-rich growth conditions, where the formation of Cu vacancies is suppressed. We computationally survey a broad suite of 23 dopants and find that only Cl and Br are effective n-type dopants. Therefore, we recommend that future experimental doping efforts utilize phase boundary mapping to optimize the electron concentration and resolve the anomalous p–n–p transitions observed in halogen-doped BiCuSeO. The prospect of n-type doping, as revealed by our defect calculations, paves the path for rational design of BiCuSeO chemical analogues with similar doping behavior and even better TE performance.more » « less
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acs.jpclett.0c03620
