Faux‐hawk fullerenes are promising candidates for high‐performance organic field‐effect transistors (OFETs). They show dense molecular packing and high thermal stability. Furthermore, in contrast to most other C60derivates, functionalization of the fullerene core by the fluorinated group C6F4CF2does not increase their lowest unoccupied orbital position, which allows the use of air‐stable molecular n‐dopants to optimize their performance. The influence of n‐doping on the performance of OFETs based on the faux‐hawk fullerene 1,9‐C60(cyclo‐CF2(2‐C6F4)) (C60FHF) is studied. An analytic model for n‐doped transistors is presented and used to clarify the origin of the increase in the subthreshold swing usually observed in doped OFETs. It is shown that the increase in subthreshold swing can be minimized by using a bulk dopant layer at the gate dielectric/C60FHF layer instead of a mixed host:dopant layer. Following an optimization of the OFETs, an average electron mobility of 0.34 cm2 V−1 s−1, a subthreshold swing below 400 mV dec−1for doped transistors, and a contact resistance of 10 kΩ cm is obtained, which is among the best performance for fullerene based n‐type semiconductors.
A new approach to control the n‐doping reaction of organic semiconductors is reported using surface‐functionalized gold nanoparticles (f‐AuNPs) with alkylthiols acting as the catalyst only upon mild thermal activation. To demonstrate the versatility of this methodology, the reaction of the n‐type dopant precursor N‐DMBI‐H with several molecular and polymeric semiconductors at different temperatures with/without f‐AuNPs, vis‐à‐vis the unfunctionalized catalyst AuNPs, was investigated by spectroscopic, morphological, charge transport, and kinetic measurements as well as, computationally, the thermodynamic of catalyst activation. The combined experimental and theoretical data demonstrate that while f‐AuNPs is inactive at room temperature both in solution and in the solid state, catalyst activation occurs rapidly at mild temperatures (~70 °C) and the doping reaction completes in few seconds affording large electrical conductivities (~10–140 S cm−1). The implementation of this methodology enables the use of semiconductor+dopant+catalyst solutions and will broaden the use of the corresponding n‐doped films in opto‐electronic devices such as thin‐film transistors, electrochemical transistors, solar cells, and thermoelectrics well as guide the design of new catalysts.
more » « less- NSF-PAR ID:
- 10522499
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Angewandte Chemie International Edition
- Volume:
- 63
- Issue:
- 33
- ISSN:
- 1433-7851
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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