Identifying high-mobility tetracene derivatives using a non-adiabatic molecular dynamics approach

The search for conductive soft matter materials with significant charge mobility at ambient con- ditions has been a major priority in organic electronics (OE) research. Alkylated tetracenes are promising cost-effective candidate molecules that can be synthesized using wet chemistry methods, resulting in columnar single crystals with pronounced structural stability at and above room temperature. A remarkable characteristic of these materials is the capability of tuning the tetracene core intracolumnar stacking pattern and crystal melting point via side chain length and type modifications. In this study, we examine the performance of a series of alkylated tetracenes as hole conducting materials using a novel atomistic simulation technique that allows us to predict both the charge transport mechanism and mobilities. Our simulations demonstrate that molec- ular wires of alkylated tetracenes are able of band-like hole conduction at room temperature, with mobility values ranging up to 21 cm2V-1s-1, thus rendering such materials a highly promis- ing choice for flexible OE applications. As regards charge transfer robustness, two promising tetracene derivatives are identified with the capability of seamless inter-wire polaron delocaliza- tion, alleviating possible transfer bottlenecks due to local molecular defects. Our findings suggest that alkylated tetracenes offer an attractive route towards flexible columnar OE materials with unprecedented hole mobilities.