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Metallo-Supramolecular Rod–Coil Block Copolymer Thin Films for Stretchable Organic Field Effect Transistor Application

Cite this: Macromolecules 2022, 55, 23, 10670–10681
Publication Date (Web):November 17, 2022
https://doi.org/10.1021/acs.macromol.2c00957
Copyright © 2022 American Chemical Society

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    Abstract

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    Herein, to decrease the synthetic burden of the rod–coil diblock copolymers, the coordination-driven self-assembly approach is utilized to readily construct a series of polystyrene (PS)-block-poly(3-hexylthiophene) (P3HT) copolymers with dynamic heteroleptic coordination bonds between the two blocks. In detail, the chain length of the PS is varied for a fixed P3HT chain length to produce block copolymers, namely, PS85–Zn–P3HT187 (P1) and PS161–Zn–P3HT187 (P2), with comparable electrical performance to that of homopolymer P3HT (P0) in the unstrained state, along with enhanced crack onset strain and much less reduced mobility under 25–100% strain. The ability to maintain the charge transport characteristics is due to the longer coil chain length and amorphous PS regions for the dissipation of strain energy. The organic field effect transistors of P2 with a longer PS segment show only a slight change in mobility from 5.48 × 10–3 to 1.40 × 10–3 cm2 V–1 s–1 under 25–100% and maintain this mobility even after being subjected to 100 repeated stretching/releasing cycles at 50% strain. This proof-of-concept demonstration of the proposed molecular engineering approach based on the metallo-supramolecular method provides a suitable route to the molecular design of stretchable polymer semiconductors with balanced mechanical and electrical behaviors.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.2c00957.

    • Materials and measurements, synthesis of polymers, 1H-NMR spectra, DSC thermograms, PESA measurements, transfer and output plots, 2D-GIXRD patterns, DMT modulus mappings and histograms, and results and discussion of PS/P3HT blending tests (PDF).

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