Abstract

2Dmolecular crystals (2DMCs) are emerging as excellent candidates for theapplication of organic field‐effect transistors (OFETs), owing to theirenhanced charge transport efficiency and long‐range molecular ordering.However, many current methods involve an additional transfer process, whichlargely hinders the large‐area fabrication of high‐quality, intact 2DMCs forpractical applications. Here, an efficient surficial Marangoni flow‐inducedself‐assembly (SMFIS) method is developed for the fabrication of 2DMCs directlyon target substrates without the need of a transfer process. This methodutilizes a solvent/antisolvent system to confine the crystallization field at aliquid/air interface, and then the formed 2DMCs land on the target substratewith the full solvent evaporation. By controlling the vertical convection flowand the spreading coefficient of the solvent/antisolvent system, few‐layer (3–4layers) 2DMCs are directly produced on the target substrates. The SMFIS methodshows no substrate dependency and universal compatibility. Withbis(triethylsilylethynyl)anthradithiophene (Dif‐TES‐ADT) as an example, theresulting 2D Dif‐TES‐ADT crystal exhibits an efficient charge transport withhigh average mobility up to 2.15 cm² V⁻¹ s⁻¹.The proposed method with general applicability has great potential to bedeveloped as a platform for the growth of high‐quality 2DMCs on the targetsubstrate.