Copper(I) thiocyanate (CuSCN) is rising to prominence as a hole‐transporting semiconductor in various opto/electronic applications. Its unique combination of good hole mobility, high optical transparency, and solution‐processability renders it a promising hole‐transport layer for solar cells and p‐type channel in thin‐film transistors. CuSCN is typically deposited from sulfide‐based solutions with diethyl sulfide (DES) being the most widely used. However, little is known regarding the effects of DES on CuSCN films despite the fact that DES can coordinate with Cu(I) and result in a different coordination polymer having a distinct crystal structure when fully coordinated. Herein, the coordination of DES in CuSCN films is thoroughly investigated with a suite of characterization techniques as well as density functional theory. This study reveals that DES directly affects the microstructure of CuSCN by stabilizing the polar crystalline surfaces via the formation of strong coordination bonds. Furthermore, a simple antisolvent treatment is demonstrated to be effective at modifying the microstructure and morphology of CuSCN films. The treatment with tetrahydrofuran or acetone leads to uniform films consisting of CuSCN crystallites with high crystallinity and their surfaces passivated by DES molecules, resulting in an increase in the hole mobility from 0.01 to 0.05 cm² V⁻¹ s⁻¹.

中文翻译：

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阐明硫氰酸铜（I）薄膜中二乙基硫分子的配位并通过反溶剂处理改善空穴传输

在各种光电/电子应用中，硫氰酸铜（I）都作为空穴传输半导体而日益突出。它具有良好的空穴迁移率，高光学透明性和溶液加工性的独特组合，使其成为用于太阳能电池和p的有希望的空穴传输层薄膜晶体管中的“类型”通道。CuSCN通常从基于硫化物的溶液中沉积，其中最广泛使用的是二乙基硫（DES）。然而，关于DES对CuSCN膜的影响知之甚少，尽管事实是DES可以与Cu（I）配位并在完全配位时产生具有独特晶体结构的不同配位聚合物。在本文中，使用一套表征技术以及密度泛函理论对CuSCN膜中DES的配位进行了彻底研究。这项研究表明，DES通过形成强配位键来稳定极性晶体表面，从而直接影响CuSCN的微观结构。此外，已证明简单的抗溶剂处理可有效改善CuSCN膜的微观结构和形态。² V ^-1 s ^-1。