Anwar Husna, Johnston Andrew, Mahesh Suhas, Singh Kamalpreet, Wang Zhibo, Kuntz Douglas A, Tamblyn Isaac, Voznyy Oleksandr, Privé Gilbert G, Sargent Edward H
The Edward S. Rogers Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada M5S 3G4.
Department of Physical and Environmental Sciences, University of Toronto Scarborough, Scarborough, Ontario, Canada M1C 1A4.
ACS Cent Sci. 2022 May 25;8(5):571-580. doi: 10.1021/acscentsci.2c00041. Epub 2022 May 6.
High-throughput experimentation (HTE) seeks to accelerate the exploration of materials space by uniting robotics, combinatorial methods, and parallel processing. HTE is particularly relevant to metal halide perovskites (MHPs), a diverse class of optoelectronic materials with a large chemical space. Here we develop an HTE workflow to synthesize and characterize light-emitting MHP single crystals, allowing us to generate the first reported data set of experimentally derived photoluminescence spectra for low-dimensional MHPs. We leverage the accelerated workflow to optimize the synthesis and emission of a new MHP, methoxy-phenethylammonium lead iodide ((4-MeO-PEAI)-PbI). We then synthesize 16 000 MHP single crystals and measure their photoluminescence to study the effects of synthesis parameters and compositional engineering on the emission intensity of 54 distinct MHPs: we achieve an acceleration factor of more than 100 times over previously reported HTE MHP synthesis and characterization methods. Using insights derived from this analysis, we screen an existing database for new, potentially emissive MHPs. On the basis of the Tanimoto similarity of the bright available emitters, we present our top candidates for future exploration. As a proof of concept, we use one of these (3,4-difluorophenylmethanamine) to synthesize an MHP which we find has a photoluminescence quantum yield of 10%.
高通量实验（HTE）旨在通过结合机器人技术、组合方法和并行处理来加速对材料空间的探索。HTE 与金属卤化物钙钛矿（MHP）特别相关，MHP 是一类具有广阔化学空间的多样化光电材料。在此，我们开发了一种 HTE 工作流程，用于合成和表征发光的 MHP 单晶，从而使我们能够生成首个关于低维 MHP 的实验得出的光致发光光谱数据集。我们利用这一加速工作流程来优化新型 MHP——甲氧基苯乙铵碘化铅（(4-MeO-PEAI)-PbI）的合成与发光性能。然后，我们合成了 16000 个 MHP 单晶并测量它们的光致发光，以研究合成参数和成分工程对 54 种不同 MHP 的发光强度的影响：与先前报道的 HTE MHP 合成和表征方法相比，我们实现了超过 100 倍的加速因子。利用从该分析中获得的见解，我们在现有数据库中筛选新的、可能发光的 MHP。基于明亮的可用发光体的谷本相似度，我们展示了未来探索的顶级候选物。作为概念验证，我们使用其中一种（3,4-二氟苯甲胺）合成了一种 MHP，我们发现其光致发光量子产率为 10%。
