First-principles calculations of electronic and optical properties of disordered and amorphous CuI-based ternary alloys

我们建议进行预测计算的透明半导体铜卤化物三元化合物和合金的电子能带结构，输运系数和光谱，使用和进一步发展最好的理论和计算方法的固体。在研究单元FOR 2857的第一阶段，我们的目标是优化p型CuI的导电性和透明度。在对γ-CuI相进行了深入研究之后，我们研究了其他晶相、不同化学计量比、缺陷和替代掺杂。我们预测和特点的新的稳定的化合物从计算的三元系统，包括铜，I和另一个元素的周期表到Bi的相图。我们的主要目标是提出在不影响透明度的情况下提高空穴迁移率和浓度的方法。在第二个供资期，我们希望在现有成果的基础上再接再厉。首先，我们将扩大搜索空间，将焦点从CuI转移到CuI基三元晶体。我们的计划包括：（i）我们已经预先选择作为有前途的p型透明半导体的CuI基三元化合物的掺杂剂的高通量工程;（ii）Cu空位和I配位的修改对CuI基晶体的电子性质的影响的深入分析;（iii）非晶三元薄膜的计算表征。第二，我们将推进三元相图的热力学分析，包括熵项，因此占无序的热力学稳定性和电子性质的CuI基合金的影响。像往常一样，我们将过滤掉不满足目标应用程序相关要求的系统。最好的候选系统将被传递到精确的电子表征超出标准的密度泛函理论（DFT），应用新的近似DFT和时间相关的DFT，我们已经从多体微扰理论。在我们计算研究的所有阶段，将相关信息持续传输给FOR 2857的合作伙伴将有助于加快工作并最大限度地发挥其影响。在整个项目期间收集的大量数据将使用机器学习进行分析，以提取p型透明导体的设计规则。

We propose to perform predictive calculations of electronic band structures, transport coefficients and optical spectra of transparent semiconducting copper-halide ternary compounds and alloys, using and further developing the best available theoretical and computational approaches for solids. In the first period of the research unit FOR2857 we targeted the optimization of conductivity and transparency of p-type CuI. After a thorough study of the zincblende phase γ-CuI, we investigated other crystalline phases, different stoichiometries, defects and substitutional doping. We predicted and characterized novel stable compounds from the calculation of phase diagrams of ternary systems including Cu, I and another element of the periodic table up to Bi. Our main objective was and remains to propose ways to enhance hole mobility and concentration without compromising transparency. In the second funding period we want to build upon present results. First, we will enlarge the search space, moving the focus from CuI to CuI-based ternary crystals. Our plan includes: (i) high-throughput engineering of dopants for CuI-based ternaries that we have pre-selected as promising p-type transparent semiconductors; (ii) deep analysis of the effect of Cu vacancies and modifications of I coordination on the electronic properties of CuI-based crystals; (iii) computational characterization of amorphous ternary films. Second, we will push forward the thermodynamic analysis of the ternary phase diagrams to include entropic terms, and therefore account for effects of disorder on thermodynamic stability and electronic properties of CuI-based alloys. As usual, we will filter out systems that do not satisfy requirements related to the targeted application. The best candidate systems will instead be passed forward for accurate electronic characterization beyond standard density-functional theory (DFT), applying new approximations for DFT and time-dependent DFT, that we have derived from many-body perturbation theory. At all stages of our computational investigation, a continuous transfer of relevant information to the partners of FOR2857 will allow to accelerate the work and maximize its impact. The large amount of data collected during the whole duration of the project will be analyzed using machine learning to extract design rules for p-type transparent conductors.