Highly Deformable Rigid Glassy Conjugated Polymeric Thin Films

Abstract

Abstract Wearable devices benefit from the use of stretchable conjugated polymers (CPs). Traditionally, the design of stretchable CPs is based on the assumption that a low elastic modulus ( E ) is crucial for achieving high stretchability. However, this research, which analyzes the mechanical properties of 65 CP thin films, challenges this notion. It is discovered that softness alone does not determine stretchability; rather, it is the degree of entanglement that is critical. This means that rigid CPs can also exhibit high stretchability, contradicting conventional wisdom. To inverstigate further, the mechanical behavior, electrical properties, and deformation mechanism of two model CPs: a glassy poly(3‐butylthiophene‐2,5‐diyl) (P3BT) with an E of 2.2 GPa and a viscoelastic poly(3‐octylthiophene‐2,5‐diyl) (P3OT) with an E of 86 MPa, are studied. Ex situ transmission X‐ray scattering and polarized UV–vis spectroscopy revealed that only the initial strain (i.e., <20%) exhibits different chain alignment mechanisms between two polymers, while both rigid and soft P3ATs showed similarly behavior at larger strains. By challenging the conventional design metric of low E for high stretchability and highlighting the importance of entanglement, it is hoped to broaden the range of CPs available for use in wearable devices.