Journal
CHEMISTRY OF MATERIALS
Volume 34, Issue 1, Pages 314-324Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c03626
Keywords
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Funding
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Science, ICT & Future Planning [2020R1A2C2008757, 2021R1A2C1007212]
- National Research Foundation of Korea [2020R1A2C2008757, 2021R1A2C1007212] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Comparative device analyses were conducted to understand charge-transport behavior in PFETs using DPP-based conjugated copolymers with chalcogenophene units. The orientation of the copolymer backbone significantly impacted the electrical performance of the PFETs, with face-on-oriented copolymers exhibiting superior mobility despite lower planarity. The degree of delocalization of disordered domains in the DPP-based polymer was found to be crucial in determining the charge-transport behavior in PFETs.
Herein, we present comparative device analyses that help understand the charge-transport behavior in polymer field-effect transistors (PFETs) in which synthesized diketopyrrolopyrrole-based (DPP-based) conjugated copolymers bearing chalcogenophene units are used as semiconducting channel materials. The copolymer backbone orientations were successfully modified by tailoring the spacer units of the conjugated copolymers to be face-on-oriented for DPP-based copolymers bearing methylthiophene-furan-methylthiophene units (PDPP-MT-F-MT) and edge-on-oriented for the corresponding thiophene (PDPP-MT-T-MT)- and selenophene (PDPP-MT-Se-MT)-containing copolymers. Higher backbone planarity and higher field-effect mobilities were expected for the edge-on-oriented DPP-based copolymers (PDPP-MT-T-MT and PDPP-MT-Se-MT) based on density functional theory calculations; however, the face-on-oriented PDPP-MT-F-MT-based PFET exhibited superior electrical performance in terms of field-effect mobility. Charge-transport analyses based on the Gaussian disorder model, focusing on the charge-transport behavior of the disordered (amorphous) domains in the DPP-based polymer films, revealed that the localized states in the disordered domains of the face-oriented PDPP-MT-F-MT become more delocalized than those of the edge-oriented PDPP-MT-T-MT and PDPP-MT-Se-MT polymers when a gate bias is applied to their PFETs. Therefore, we attribute the electrical performance of a DPP-based PFET to the degree of delocalization of the disordered domains of its DPP-based polymer, which has a significant impact on the charge-transport behavior.
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