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Printing 2D Conjugated Polymer Monolayers and Their Distinct Electronic Properties
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-02-06 , DOI: 10.1002/adfm.201909787 Prapti Kafle 1 , Fengjiao Zhang 1 , Noah B. Schorr 2 , Kai‐Yu Huang 1 , Joaquín Rodríguez‐López 2 , Ying Diao 1
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-02-06 , DOI: 10.1002/adfm.201909787 Prapti Kafle 1 , Fengjiao Zhang 1 , Noah B. Schorr 2 , Kai‐Yu Huang 1 , Joaquín Rodríguez‐López 2 , Ying Diao 1
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Recently, 2D monolayer films of conjugated polymers have gained increasing attention owing to the preeminence of 2D inorganic films that exhibit unique optoelectronic and mechanical properties compared to their bulk analogs. Despite numerous efforts, crystallization of semiconducting polymers into highly ordered 2D monolayer films still remains challenging. Herein, a dynamic‐template‐assisted meniscus‐guided coating is utilized to fabricate continuous, highly ordered 2D monolayer films of conjugated polymers over a centimeter scale with enhanced backbone π–π stacking. In contrast, monolayer films printed on solid substrates confer upon the 1D fiber networks strong alkyl side‐chain stacking at the expense of backbone packing. From single‐layers to multilayers, the polymer π‐stacks change from edge‐on to bimodal orientation as the film thickness reaches ≈20 nm. Spectroscopic and cyclic voltammetry analysis reveals an abrupt increase in J‐aggregation and absorption coefficient and a decrease in bandgap and highest occupied molecular orbital level until critical thickness, possibly arising from the straightened polymer backbone. This is corroborated by an abrupt increase in hole mobility with film thickness, reaching a maximum of 0.7 cm2 V−1 s−1 near the critical thickness. Finally, fabrication of chemical sensors incorporating polymer films of various thicknesses is demonstrated, and an ultrahigh sensitivity of the ≈7 nm thick ultrathin film (bilayers) to 1 ppb ammonia is shown.
中文翻译：
印刷二维共轭聚合物单分子膜及其独特的电子性能
最近，由于2D无机膜比其本体类似物表现出独特的光电和机械性能，因此共轭聚合物的2D单层膜受到越来越多的关注。尽管做出了许多努力，将半导体聚合物结晶成高度有序的2D单层膜仍然具有挑战性。本文中，利用动态模板辅助的弯月面引导涂层来制造连续的，高度有序的二维共轭聚合物二维单层膜，并具有增强的骨架π-π堆叠能力。相反，印在固体基材上的单层薄膜赋予一维纤维网络以牢固的烷基侧链堆叠的功能，而牺牲了骨架的堆积。从单层到多层 当膜厚度达到≈20nm时，聚合物的π堆叠从边沿到双峰方向发生变化。光谱和循环伏安法分析显示，直到临界厚度为止，J聚集和吸收系数突然增加，带隙和最高占据分子轨道能级下降，这可能是由于聚合物主链变直引起的。空穴迁移率随膜厚的突然增加而得到证实，最大值达到0.7 cm临界厚度附近为2 V -1 s -1。最后，展示了结合了各种厚度的聚合物膜的化学传感器的制造，并显示了≈7nm厚的超薄膜（双层）对1 ppb氨水的超高灵敏度。
更新日期：2020-03-19
中文翻译：
印刷二维共轭聚合物单分子膜及其独特的电子性能
最近，由于2D无机膜比其本体类似物表现出独特的光电和机械性能，因此共轭聚合物的2D单层膜受到越来越多的关注。尽管做出了许多努力，将半导体聚合物结晶成高度有序的2D单层膜仍然具有挑战性。本文中，利用动态模板辅助的弯月面引导涂层来制造连续的，高度有序的二维共轭聚合物二维单层膜，并具有增强的骨架π-π堆叠能力。相反，印在固体基材上的单层薄膜赋予一维纤维网络以牢固的烷基侧链堆叠的功能，而牺牲了骨架的堆积。从单层到多层 当膜厚度达到≈20nm时，聚合物的π堆叠从边沿到双峰方向发生变化。光谱和循环伏安法分析显示，直到临界厚度为止，J聚集和吸收系数突然增加，带隙和最高占据分子轨道能级下降，这可能是由于聚合物主链变直引起的。空穴迁移率随膜厚的突然增加而得到证实，最大值达到0.7 cm临界厚度附近为2 V -1 s -1。最后，展示了结合了各种厚度的聚合物膜的化学传感器的制造，并显示了≈7nm厚的超薄膜（双层）对1 ppb氨水的超高灵敏度。
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