Dynamic processes in transient phases during self-assembly of organic semiconductor thin films
Dynamic processes in transient phases during self-assembly of organic semiconductor thin films
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有机半导体薄膜自组装过程中瞬态动态过程
DOI：
10.1039/d1me00078k
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发表时间：
2022
影响因子：
3.6
通讯作者：
Headrick, Randall L.
中科院分区：
文献类型：
--
作者：
Wan, Jing;Li, Yang;Benson, Jared;Miller, Richards;Zhernenkov, Mikhail;Freychet, Guillaume;Headrick, Randall L.
无论是基础研究还是制备具有近本征电荷传输特性的有机薄膜，理解和控制结晶过程一直是溶液法制备有机薄膜的重要挑战。报道了2-decyl-7-phenyl-[1]benzothieno[3，2-b][1]benzothiophene(Ph-BTBT-C10)从溶液中析出过程中的原位X射线散射研究。在近晶-E/晶界以下的温度下，结晶在到达最终的稳定晶相之前经历了一个短暂的液晶状态。显著的动力学发生在转变的最初几秒钟，这是通过X射线散射强度的波动观察到的，并与瞬时薄膜与蒸发溶剂共存的时间间隔相关。在这些条件下，向稳定晶相的转变需要几分钟甚至几个小时，这可能是由于分子的不对称性造成的。过渡相具有潜在的应用价值，因为它们可以作为有机薄膜自组装的途径。然而，我们的观察表明，长寿命的单层堆积中间态并不作为双层堆积晶相的模板。相反，通过成核来取代颗粒结构，其中成核自由能势垒与阻止分子将其长轴反转180°的势垒有关。
Understanding and manipulating crystallization processes has been an important challenge for solution-processed organic thin films, both for fundamental studies and for fabricating thin films with near-intrinsic charge transport properties. We report an in situ X-ray scattering study of the crystallization of 2-decyl-7-phenyl-[1]benzothieno[3,2-b][1]benzothiophene (Ph-BTBT-C10) during its deposition from solution. At temperatures modestly below the smectic-E/crystalline phase boundary, the crystallization goes through a transient liquid crystal state before reaching the final stable crystalline phase. Significant dynamics occur in the first few seconds of the transition, which are observed through fluctuations in the X-ray scattering intensity, and are correlated with the time interval that the transient thin film coexists with the evaporating solvent. The transition to the stable crystalline phase takes minutes or even hours under these conditions, which may be a result of the asymmetry of the molecule. Transient phases are of potential interest for applications, since they can act as a route to self-assembly of organic thin films. However, our observations show that the long-lived monolayer-stacked intermediate state does not act as a template for the bilayer-stacked crystalline phase. Rather, the grain structure is replaced through nucleation, where the nucleation free-energy barrier is related to a potential barrier that prevents molecules to flip their long axis by 180°.
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DOI：
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DOI：
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发表时间：
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