The newly emerging field in organic electronics is to control the molecule–substrate interface properties at a two-dimensional (2D) limit via interfacial interactions, which paves the way for driving the molecular assembly for highly ordered 2D molecular crystalline films with precise molecular layers and large-area uniformity. Here, by exploiting molecule–substrate van der Waals (vdW) interactions, we demonstrate thermally induced self-assembly of 2D organic crystalline films exhibiting well-defined molecular layer number over a millimeter-sized area. The organic field-effect transistors (OFETs) with bilayer films show excellent electrical performance with a maximum mobility of 12.8 cm² V^–1 s^–1. Moreover, we find that the monolayer films can act as interfacial molecular templates to construct heterojunctions with well-balanced ambipolar transport behaviors. The capability of thermally induced self-assembly of 2D molecular crystalline films with controllable molecular layers and scale-up coverage opens up a way for realizing complicated electronic applications, such as lateral heterojunctions and superlattices.

中文翻译：

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通过界面相互作用调制的自组装，具有精确定义的分子层的毫米尺寸二维分子晶体半导体

有机电子学的新兴领域是通过界面相互作用将分子-底物的界面特性控制在二维（2D）极限，这为驱动具有精确分子层的高度有序的2D分子晶体膜的分子组装铺平了道路。大面积均匀性。在这里，通过利用分子与底物的范德华力（vdW）相互作用，我们证明了热诱导的2D有机晶体薄膜的自组装，该薄膜在毫米大小的区域内显示出明确定义的分子层数。具有双层薄膜的有机场效应晶体管（OFET）具有出色的电气性能，最大迁移率为12.8 cm ² V ^–1 s ^–1。此外，我们发现单层膜可以充当界面分子模板，以构建具有良好平衡的双极传输行为的异质结。具有可控分子层和按比例放大覆盖率的2D分子晶体薄膜的热诱导自组装能力为实现复杂的电子应用（例如横向异质结和超晶格）开辟了道路。