Aromatic Size Engineering in Glycolated N-type Semiconducting Polymers Enables High performance Organic Electrochemical Transistors

Maryam Alsufyani^a, Reem Rashid^b, Karl Thorley^c, Ruiheng Wu^b, Xingxing Chen^d, Jonathan Rivnay^b, Iain McCulloch^a

^aDepartment of Chemistry, University of Oxford, UK, Mansfield Rd, Oxford, United Kingdom

^bDepartment of Biomedical Engineering, Northwestern University, 2145 Sheridan Road, Evanston, United States

^cDepartment of Chemistry, University of Kentucky, 125 Chemistry/Physics Building, Lexington

^dKing Abdullah University of Science and Technology, Physical Sciences and Engineering Division, KAUST Solar Center, 23955, Thuwal, Saudi Arabia

Proceedings of Organic Bioelectronics Conference 2022 (OBe2022)

Online, Spain, 2022 February 8th - 9th

Organizers: Christopher Proctor, Maria Asplund and Mary Donahue

Poster, Maryam Alsufyani, 006
Publication date: 14th January 2022

ePoster:

Three fused electron-deficient semiconducting polymers are deliberately designed to overcome major limitations (e.g. electron mobility, electrical conductivity, and air stability) of recently emerging n-type electronic functional devices, such as organic electrochemical transistors (OECTs). Our molecular design criteria show that increasing the density of the electron-withdrawing lactone functional group along the backbone, through a systematic reduction in the aromatic ring content, can play a major role in optimizing OECT performance, especially when combined with the rigidly locked conformation imposed by aldol condensation. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the phenyl acene content from 0% phenyl (P-0), to 50% (P-50), and 75% (P-75) resulted in progressively larger electron affinities (up to -4.37 eV). When electrochemically doped in OECT devices. Remarkable OECT electron mobility (µe) of up to 0.15 cm2 V-1 s-1 and volumetric capacitance (C*) as high as 98.4 F cm-3, were recorded simultaneously. As a result, P-75- based OECT delivers a record-high maximum geometry-normalized transconductance of 5.5 S cm-1 and a maximum µC* product of 14.8 F cm-1 V-1 s-1. The µC* figure of merit and OECT electron mobility (µe) are more than one order of magnitude higher than that of the state-of-the-art n-type OECTs. These results demonstrate this class of fused electron-deficient polymers as promising n-doped OECT materials, which advances the broader organic electronic field, expanding the limited library of n-type OECT materials. Our results support the role of chemical design in the performance of n-type polymer semiconductors and provide new insights into the molecular design guidelines for the next generation of high-performance n-type OECT materials and the broader materials field.

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