Design Rules for Transparent Push–Pull Electron Acceptors: A Case Study on Perylenediimide Derivatives

• Published in: The journal of physical chemistry letters Vol. 11; no. 21; pp. 9265 - 9271
• Main Authors: Carter, Ki-Jana B, Grossman, Jeffrey C
• Format: Journal Article
• Language: English
• Published: American Chemical Society 05.11.2020
• Subjects: Physical Insights into Materials and Molecular Properties
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/acs.jpclett.0c02485

Transparent photovoltaics are receiving increased attention for their wide range of applicability, but there have been few attempts to systematically tune organic materials to achieve transparency. In this Letter, we study the influence of simple structural modifications on the photoabsorption spectrum of the nonfullerene electron acceptor perylenediimide. Motivated by push–pull design strategies, we explore the effects of applying electron-donating functional groups with varying strengths using three design motifs. We demonstrate that relative Mulliken electronegativity, which can be easily computed using an optimally tuned screened range-separated hybrid functional, is a useful metric for finding suitable donor groups. We also demonstrate that donor groups that include a conjugated spacer are crucial to obtaining a planar molecule with uniform conjugation and low-energy charge-transfer excitations. These simple design rules can be used to design near-infrared absorbing transparent electron acceptors based on perylenediimide and other promising molecular platforms.