混合过氧化物的物理驱动发现和带隙工程学

IF 6.2 Q1 CHEMISTRY, MULTIDISCIPLINARY
Sheryl L. Sanchez, Elham Foadian, Maxim Ziatdinov, Jonghee Yang, Sergei V. Kalinin, Yongtao Liu and Mahshid Ahmadi
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引用次数: 0

摘要

混合型过氧化物的独特之处在于其可调谐性,可以通过置换实现带隙工程。从应用的角度来看,这允许在包晶石和硅或两种或多种包晶石之间创建串联电池,从而提高效率,超越单结肖克利-奎塞尔极限。然而,混合型包光体固溶体的光带隙与浓度的关系可能是非线性的,甚至是非单调的,这是由内部成员之间的带排列、缺陷态和乌尔巴赫尾的存在以及相分离决定的。探索新成分带来的共同问题是:发现具有理想带隙的成分,以及建立带隙浓度依赖性的物理模型。在此,我们报告了基于结构化高斯过程(sGP)模型和定制 sGP(c-sGP)的实验工作流程的开发情况,该流程允许联合发现实验行为和基础物理模型。这种方法通过具有已知地面实况的模拟数据集进行了验证,发现它能加速发现实验行为和基础物理模型。d/c-sGP 方法利用几个计算出的薄膜带隙数据点来指导有针对性的探索,最大限度地减少了薄膜制备步骤的数量。通过迭代探索,我们证明了结合 5 个带隙模型的 c-sGP 算法收敛迅速,揭示了 MA1-xGAxPb(I1-xBrx)3 带隙图中的关系。 这种方法为有效理解二元体系中带隙浓度依赖性的物理模型提供了一种很有前途的方法,这种方法还可以扩展到三元或更高维的体系。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Physics-driven discovery and bandgap engineering of hybrid perovskites†

Physics-driven discovery and bandgap engineering of hybrid perovskites†

Physics-driven discovery and bandgap engineering of hybrid perovskites†

The unique aspect of hybrid perovskites is their tunability, allowing the engineering of the bandgap via substitution. From the application viewpoint, this allows creation of tandem cells between perovskites and silicon, or two or more perovskites, with associated increase of efficiency beyond the single-junction Shockley–Queisser limit. However, the concentration dependence of the optical bandgap in hybrid perovskite solid solutions can be non-linear and even non-monotonic, as determined by band alignments between endmembers, presence of defect states and Urbach tails, and phase separation. Exploring new compositions brings forth the joint problem of the discovery of the composition with the desired band gap and establishing the physical model of the band gap concentration dependence. Here we report the development of the experimental workflow based on structured Gaussian Process (sGP) models and custom sGP (c-sGP) that allow the joint discovery of the experimental behavior and the underpinning physical model. This approach is verified with simulated datasets with known ground truth and was found to accelerate the discovery of experimental behavior and the underlying physical model. The d/c-sGP approach utilizes a few calculated thin film bandgap data points to guide targeted explorations, minimizing the number of thin film preparation steps. Through iterative exploration, we demonstrate that the c-sGP algorithm that combined 5 bandgap models converges rapidly, revealing a relationship in the bandgap diagram of MA1−xGAxPb(I1−xBrx)3. This approach offers a promising method for efficiently understanding the physical model of band gap concentration dependence in binary systems, and this method can also be extended to ternary or higher dimensional systems.

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2.80
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