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Lyotropic Liquid Crystalline Mesophase Governs Interfacial Molecular Orientation of Conjugated Polymer Thin Films
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-06-24 , DOI: 10.1021/acs.chemmater.0c01402 Ge Qu 1 , Kyung Sun Park 1 , Prapti Kafle 1 , Fengjiao Zhang 2 , Justin J. Kwok 3 , Bijal B. Patel 1 , Detlef-M. Smilgies 4 , Lars Thomsen 5 , Christopher R. McNeill 6 , Ying Diao 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-06-24 , DOI: 10.1021/acs.chemmater.0c01402 Ge Qu 1 , Kyung Sun Park 1 , Prapti Kafle 1 , Fengjiao Zhang 2 , Justin J. Kwok 3 , Bijal B. Patel 1 , Detlef-M. Smilgies 4 , Lars Thomsen 5 , Christopher R. McNeill 6 , Ying Diao 1
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Interfacial out-of-plane molecular orientation critically influences the electronic performance of organic semiconductor thin films. The appearance of a lyotropic liquid crystalline (LC) mesophase during solution coating of conjugated polymers may directly determine the interfacial out-of-plane molecular orientation. However, a lack of studies on the packing structure of the liquid crystalline mesophase and its evolution to the solid state impedes the general understanding of the molecular orientation transformation from the liquid crystalline mesophase to solid-state thin films. This work addresses this unanswered question using poly[[2,5-bis(2-octadecyl)-2,3,5,6-tetrahydro-3,6-diketopyrrolo[3,4-c]pyrrole-1,4-diyl]-alt-(2-octylnonyl)-2,1,3-benzotriazole] (DPP-BTz) as a model compound. From near-edge X-ray adsorption fine structure spectroscopy and grazing incidence wide-angle X-ray scattering (GIWAXS) measurements, we observe distinct edge-on orientation at the top interface compared to a primarily face-on orientation in the bulk in solution-coated DPP-BTz thin films. Interestingly, the interfacial orientations in thin films are strongly correlated with those of the lyotropic liquid crystalline mesophase of DPP-BTz appearing during solution coating. Specifically, the LC mesophase adopts an edge-on orientation near the air–liquid interface and a face-on orientation in the bulk liquid layer. The multiscale structure and interfacial orientation of the mesophase are characterized by solution-state small-angle X-ray scattering and in situ GIWAXS measurements. We attribute the edge-on LC orientation at the top interface to surface energy minimization of alkyl side chains with air, while the anisotropic broad LC orientation distribution in the bulk arises from twisted molecular packing in the LC mesophase. The out-of-plane molecular orientation is preserved in the LC mesophase and is carried over to the solid-state thin film, creating the distinct edge-on interfacial alignment at the thin-film top surface.
中文翻译：
溶致液晶中间相控制共轭聚合物薄膜的界面分子取向。
界面平面外分子取向严重影响有机半导体薄膜的电子性能。共轭聚合物溶液涂布期间溶致液晶（LC）中间相的出现可能直接决定界面平面外分子取向。然而，缺乏对液晶中间相的堆积结构及其向固态的演变的研究，阻碍了对从液晶中间相到固态薄膜的分子取向转变的普遍理解。这项工作使用聚[[2,5-双（2-十八烷基）-2,3,5,6-四氢-3,6-二酮吡咯并[3,4- c ]吡咯-1,4-二基解决了这个悬而未决的问题。] -alt-（2-辛基壬基）-2,1,3-苯并三唑]（DPP-BTz）作为模型化合物。通过近边缘X射线吸附精细结构光谱学和掠射入射广角X射线散射（GIWAXS）测量，我们观察到在顶部界面中，与在溶液中的主体中的主要面向正面的方向相比，独特的面向边缘的方向涂层的DPP-BTz薄膜。有趣的是，薄膜中的界面取向与溶液涂布过程中出现的DPP-BTz的溶致液晶中间相的界面取向密切相关。具体而言，LC中间相在气液界面附近采用边沿取向，而在本体液体层中采用面对面取向。中间相的多尺度结构和界面取向通过溶液态小角度X射线散射和原位GIWAXS测量来表征。我们将在顶部界面处的边沿LC取向归因于烷基侧链与空气的表面能最小化，而各向异性的宽LC取向分布在整体中是由于LC中间相中扭曲的分子堆积引起的。平面外分子取向保留在LC中间相中，并延续到固态薄膜上，从而在薄膜顶表面产生了独特的边对界面取向。
更新日期：2020-07-28
中文翻译：
溶致液晶中间相控制共轭聚合物薄膜的界面分子取向。
界面平面外分子取向严重影响有机半导体薄膜的电子性能。共轭聚合物溶液涂布期间溶致液晶（LC）中间相的出现可能直接决定界面平面外分子取向。然而，缺乏对液晶中间相的堆积结构及其向固态的演变的研究，阻碍了对从液晶中间相到固态薄膜的分子取向转变的普遍理解。这项工作使用聚[[2,5-双（2-十八烷基）-2,3,5,6-四氢-3,6-二酮吡咯并[3,4- c ]吡咯-1,4-二基解决了这个悬而未决的问题。] -alt-（2-辛基壬基）-2,1,3-苯并三唑]（DPP-BTz）作为模型化合物。通过近边缘X射线吸附精细结构光谱学和掠射入射广角X射线散射（GIWAXS）测量，我们观察到在顶部界面中，与在溶液中的主体中的主要面向正面的方向相比，独特的面向边缘的方向涂层的DPP-BTz薄膜。有趣的是，薄膜中的界面取向与溶液涂布过程中出现的DPP-BTz的溶致液晶中间相的界面取向密切相关。具体而言，LC中间相在气液界面附近采用边沿取向，而在本体液体层中采用面对面取向。中间相的多尺度结构和界面取向通过溶液态小角度X射线散射和原位GIWAXS测量来表征。我们将在顶部界面处的边沿LC取向归因于烷基侧链与空气的表面能最小化，而各向异性的宽LC取向分布在整体中是由于LC中间相中扭曲的分子堆积引起的。平面外分子取向保留在LC中间相中，并延续到固态薄膜上，从而在薄膜顶表面产生了独特的边对界面取向。
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