论文标题
离子液体中的边界轨道和准粒子能级
Frontier Orbitals and Quasiparticle Energy Levels in Ionic Liquids
论文作者
论文摘要
室温离子液体在许多技术应用中起着重要作用，需要对其前沿分子轨道详细了解，以优化界面屏障，相对于电子注入和去除的界面屏障，反应性和稳定性。在这项工作中，我们使用GW近似中的第一原原多体基理论计算离子液体的准粒子能级，并将我们的结果与各种均值场方法进行比较，包括半遗传和混合密度和杂交密度功能理论和Hartree-Fock。我们发现，平均场结果在定性和定量上取决于交换相关效应的处理，而GW计算产生的结果与气相离子对和离子液体的实验光电谱非常吻合。这些结果将GW方法确立为理解离子液体电子结构的宝贵工具。
Room temperature ionic liquids play an important role in many technological applications and a detailed understanding of their frontier molecular orbitals is required to optimize interfacial barriers, reactivity and stability with respect to electron injection and removal. In this work, we calculate quasiparticle energy levels of ionic liquids using first-principles many-body perturbation theory within the GW approximation and compare our results to various mean-field approaches, including semilocal and hybrid density-functional theory and Hartree-Fock. We find that the mean-field results depend qualitatively and quantitatively on the treatment of exchange-correlation effects, while GW calculations produce results that are in excellent agreement with experimental photoelectron spectra of gas phase ion pairs and ionic liquids. These results establish the GW approach as a valuable tool for understanding the electronic structures of ionic liquids.
