Intrinsically Stretchable Polymer Semiconductors with Good Ductility and High Charge Mobility through Reducing the Central Symmetry of the Conjugated Backbone Units

Abstract

Intrinsically stretchable polymer semiconductors are highly demanding for flexible electronics. However, it still remains challenging to achieve synergy between intrinsic stretchability and charge transport property properly for polymer semiconductors. In this paper, terpolymers are reported as intrinsically stretchable polymeric semiconductors with good ductility and high charge mobility simultaneously by incorporation of non‐centrosymmetric spiro[cycloalkane‐1,9′‐fluorene] (spiro‐fluorene) units into the backbone of diketopyrrolopyrrole (DPP) based conjugated polymers. The results reveal that these terpolymers show obviously high crack onset strains and their tensile moduli are remarkably reduced, by comparing with the parent DPP‐based conjugated polymer without spiro‐fluorene units. They exhibit simultaneously high charge mobilities (>1.0 cm2 V−1 s−1) at 100% strain and even after repeated stretching and releasing cycles for 500 times under 50% strain. The terpolymer P2, in which cyclopropane is linked to the spiro‐fluorene unit, is among the best reported intrinsically stretchable polymer semiconductors with record mobility up to 3.1 cm2 V−1 s−1 at even 150% strain and 1.4 cm2 V−1 s−1 after repeated stretching and releasing cycles for 1000 times.

Achieving High Performance Stretchable Conjugated Polymers via Donor Structure Engineering

“…With the increasing demand for embeddable, portable, highly sensitive, and real-time monitoring medical devices, stretchable DOI: 10.1002/marc.202300169 electronic components have attracted particular interest for application in such devices. [1][2][3] Conjugated polymers have emerged as the next generation of semiconductor layer materials for stretchable electronic components, among which donor-acceptor (D-A) conjugated polymers have received special attention due to their efficient carrier mobility. [4][5][6] However, the backbone of D-A conjugated polymers are mainly composed of aromatic rings, which are highly rigid and semicrystalline, and thus are unfavorable for the mechanical ductility of the films.…”

Nature-Inspired Semiconducting Polymers with Peptide Conjugation Breakers for Intrinsically Stretchable and Self-Healable Transistors

“…Intrinsically stretchable polymers, which are achieved through deliberate molecular engineering, hold a potential alternative for overcoming these issues. Researchers have utilized various molecular designs in both backbone and side-chain engineering, such as metal–ligand bonds, hydrogen bonds, − carbosilanes, and terpolymerization without conjugation breaking − to induce intrinsic stretchability. However, the main challenges impeding the advancement of intrinsically stretchable polymer semiconductors are the limited availability of varied molecular designs and the inefficiency of laborious synthesis techniques.…”

High-Performance n-Type Stretchable Semiconductor Blends for Organic Thin-Film Transistors and Artificial Synapses

“…Provided the realization of both, additional functions can be expected to be introduced into the corresponding high-performance devices. For example, organic thin film transistors (OTFTs), as the elementary units for organic circuits, not only are the proper devices to characterize the electrical properties of semiconductors − but also can behave as electrical synapses to emulate biological memory functions. ,− Successful construction of such devices will allow for simplified learning scheme in biomimetic neuromorphic systems, without complex synchronization algorithms in practical applications. − …”