Adeniran Olugbenga, Liu Zhen-Fei
Department of Chemistry, Wayne State University, Detroit, Michigan 48202, USA.
J Chem Phys. 2021 Dec 7;155(21):214702. doi: 10.1063/5.0072995.
Interfaces formed between monolayer transition metal dichalcogenides and (metallo)phthalocyanine molecules are promising in energy applications and provide a platform for studying mixed-dimensional molecule-semiconductor heterostructures in general. An accurate characterization of the frontier energy level alignment at these interfaces is key in the fundamental understanding of the charge transfer dynamics between the two photon absorbers. Here, we employ the first-principles substrate screening GW approach to quantitatively characterize the quasiparticle electronic structure of a series of interfaces: metal-free phthalocyanine (HPc) adsorbed on monolayer MX (M = Mo, W; X = S, Se) and zinc phthalocyanine (ZnPc) adsorbed on MoX (X = S, Se). Furthermore, we reveal the dielectric screening effect of the commonly used α-quartz (SiO) substrate on the HPc:MoS interface using the dielectric embedding GW approach. Our calculations furnish a systematic set of GW results for these interfaces, providing the structure-property relationship across a series of similar systems and benchmarks for future experimental and theoretical studies.
单层过渡金属二卤化物与（金属）酞菁分子之间形成的界面在能源应用方面很有前景，并且总体上为研究混合维度的分子 - 半导体异质结构提供了一个平台。准确表征这些界面处的前沿能级排列是深入理解这两种双光子吸收体之间电荷转移动力学的关键。在此，我们采用第一性原理衬底筛选GW方法来定量表征一系列界面的准粒子电子结构：无金属酞菁（HPc）吸附在单层MX（M = Mo，W；X = S，Se）上以及锌酞菁（ZnPc）吸附在MoX（X = S，Se）上。此外，我们使用介电嵌入GW方法揭示了常用的α - 石英（SiO）衬底对HPc:MoS界面的介电屏蔽效应。我们的计算为这些界面提供了一组系统的GW结果，给出了一系列相似系统的结构 - 性质关系，并为未来的实验和理论研究提供了基准。
