Tuning the Mechanical Properties of a Polymer Semiconductor by Modulating Hydrogen Bonding Interactions

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Conjugation breakers (CBs) with different H-bonding chemistries and linker flexibilities are designed and incorporated into a diketopyrrolopyrrole (DPP)-based conjugated polymer backbone. The effects of H-bonding interactions on polymer semiconductor morphology, mechanical properties, and electrical performance are systematically investigated. We observe that CBs with an H-bonding self-association constant >0.7 or a denser packing tendency are able to induce higher polymer chain aggregation and crystallinity in as-casted thin films, resulting in a higher modulus and crack on-set strain. Additionally, the rDoC (relative degree of crystallinity) of the stretched thin film with the highest crack on-set strain only suffers a small decrease, suggesting the main energy dissipation mechanism is the breakage of H-bonding interactions. By contrast, other less stretchable polymer films dissipate strain energy through the breakage of crystalline domains, indicated by a drastic decrease in rDoC. Furthermore, we evaluate their electrical performances under mechanical strain in fully stretchable field-effect transistors. The polymer with the highest crack on-set strain has the least degradation in mobility as a function of strain. Overall, these observations suggest that we can aptly tune the mechanical properties of a polymer semiconductor by modulating intermolecular interactions, such as H-bonding chemistry and linker flexibility. Such understanding provides molecular design guidelines for future stretchable semiconductors.
Publisher
AMER CHEMICAL SOC
Issue Date
2020-07
Language
English
Article Type
Article
Citation

CHEMISTRY OF MATERIALS, v.32, no.13, pp.5700 - 5714

ISSN
0897-4756
DOI
10.1021/acs.chemmater.0c01437
URI
http://hdl.handle.net/10203/275828
Appears in Collection
MS-Journal Papers(저널논문)
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