Ahmed Faruk, Ortega-Castro Joaquín, Frontera Antonio, Mir Mohammad Hedayetullah
Department of Chemistry, Aliah University, New Town, Kolkata 700 156, India.
Dalton Trans. 2021 Jan 7;50(1):270-278. doi: 10.1039/d0dt03868g. Epub 2020 Dec 10.
Coordination polymers (CPs) in recent times have emerged as active constituents in many semiconductor devices like light emitting diodes (LED), field effect transistors (FET), photovoltaic devices and Schottky barrier diodes. An intelligent choice of linkers, careful selection of metal ions and post synthetic modification (PSM) can provide a better pathway for charge transportation. However, a proper understanding of the charge transport mechanism in CPs is still inadequate due to the lack of considerable experimental and theoretical work. In this paper, we address the theoretical elucidation of semiconducting properties and a probable pathway for charge transportation in three of our previously published CPs using density functional theory (DFT). These results help us to recognize the orbitals that have major contributions in the formation of the valence band and also provide the most likely pathway for optimum electronic communication. In this regard, the role of hydrogen bonding and unpaired electrons of metal d-orbitals is also established.
近年来，配位聚合物（CPs）已成为许多半导体器件（如发光二极管（LED）、场效应晶体管（FET）、光伏器件和肖特基势垒二极管）中的活性成分。智能选择连接体、精心挑选金属离子以及进行后合成修饰（PSM）可为电荷传输提供更好的途径。然而，由于缺乏大量的实验和理论研究，对CPs中电荷传输机制的恰当理解仍然不足。在本文中，我们使用密度泛函理论（DFT）对我们之前发表的三种CPs的半导体性质进行理论阐释，并探讨电荷传输的可能途径。这些结果有助于我们识别对价带形成有主要贡献的轨道，还能提供最有可能实现最佳电子通信的途径。在这方面，氢键和金属d轨道未成对电子的作用也得以确定。
