CAREER: Guiding automated synthesis of hybrid perovskites towards stability via knowledge of nanoscale ionic mechanisms

职业：通过纳米级离子机制的知识指导杂化钙钛矿的自动化合成以实现稳定性

• 批准号: 2043205
• 负责人: Mahshid Ahmadi
• 金额: $ 56.07万
• 依托单位: University of Tennessee Knoxville
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-06-01 至 2026-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2043205&HistoricalAwards=false
• 关键词: CAREER; Guiding; automated; synthesis; hybrid

Metal halide perovskites are a new class of hybrid materials with inorganic and organic components with the potential to revolutionize optoelectronic technologies. They have shown particular promise for the next generation of inexpensive, efficient solar cells. The primary limiting factor to widespread use of perovskites is that they are not stable in devices. This project will develop an understanding of the fundamental and specific properties of perovskites with an overarching goal of improved stability. This project will elucidate and describe the electrochemistry of these materials to inform development of new processes for manufacture of stable perovskites. This work is made possible by an innovative automated synthesis approach that allows for experimentation on a diverse range of novel compositions that would be difficult to identify and study otherwise. The PI will strive to increase interest and participation of women in materials science and engineering research careers through an active, project-based outreach program. This program will include individualized career awareness mentoring for high school students and undergraduates.Organic–inorganic halide perovskites (OIHP) have many qualities that are ideal for optoelectronic applications and are used to improve function and reduce cost of solar cells, photodetectors, and light-emitting diodes. The substantive hurdles to widespread, commercial use of OIHPs are their instability and low long-term performance. Precise control of ionic chemistry and understanding of how interfacial and surface chemistry affects function are essential to overcome these limitations. This project will measure and describe the underlying mechanisms that affect OIHP intrinsic stability to create predictive models that will inform design of durable materials. The three challenges related to the stability of OIHPs examined in this project are: 1) establish rapid guided automated combinatorial synthesis workflow for material discovery and optimization, 2) determine the role of ion chemistry via electrochemical gating experiments, and 3) describe the kinetics and thermodynamics of the interfacial electrochemical processes on the three-phase junctions. The project will employ microscopy techniques and imaging of in-operando devices to build a comprehensive understanding of the internal electrochemical functionality of OIHP systems, which would enable a path toward predictive modelling and optimization of processing. The proposed automated synthesis approach using rapid characterization and slow device testing will allow for navigation of the compositional and processing space of these materials. The project-based outreach program will integrate the physics of electronic and ionic charge transports with machine learning concepts for new research experiences for undergraduate and graduate students. Grade-level appropriate versions of these activities will be offered to interested female high school students to increase interest in and improve preparation for materials science careers for women and other groups underrepresented in STEM.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

金属卤化物钙钛矿是一类具有无机和有机组分的新型混合材料，具有革新光电技术的潜力。它们在下一代廉价、高效的太阳能电池方面表现出了特别的前景。钙钛矿广泛使用的主要限制因素是它们在设备中不稳定。该项目将发展对钙钛矿的基本和具体性质的理解，其总体目标是提高稳定性。该项目将阐明和描述这些材料的电化学，以告知制造稳定钙钛矿的新工艺的开发。这项工作是通过一种创新的自动化合成方法实现的，该方法允许对各种难以识别和研究的新型组合物进行实验。PI将通过积极的、基于项目的推广计划，努力提高妇女对材料科学和工程研究事业的兴趣和参与。该计划将包括针对高中生和本科生的个性化职业意识辅导。有机-无机卤化物钙钛矿（OIHP）具有许多光电应用的理想品质，可用于改善太阳能电池，光电探测器和发光二极管的功能并降低成本。OIHP广泛商业应用的实质性障碍是其不稳定性和低长期性能。精确控制离子化学和了解界面和表面化学如何影响功能对于克服这些限制至关重要。该项目将测量和描述影响OIHP内在稳定性的潜在机制，以创建预测模型，为耐用材料的设计提供信息。本项目中研究的与OIHP稳定性相关的三个挑战是：1）建立快速引导的自动化组合合成工作流程，用于材料发现和优化，2）通过电化学门控实验确定离子化学的作用，以及3）描述动力学和热力学三相结上界面电化学过程。该项目将采用显微镜技术和操作中设备的成像，以全面了解OIHP系统的内部电化学功能，这将有助于预测建模和优化处理。所提出的自动化合成方法，使用快速表征和缓慢的设备测试将允许这些材料的组成和处理空间的导航。基于项目的外展计划将电子和离子电荷传输的物理学与机器学习概念相结合，为本科生和研究生提供新的研究经验。将向感兴趣的女高中生提供这些活动的年级适当版本，以提高妇女和其他在STEM中代表性不足的群体对材料科学职业的兴趣并改善其准备。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

项目成果

Unraveling the hysteretic behavior at double cations-double halides perovskite - electrode interfaces

• DOI: 10.1016/j.nanoen.2021.106428
• 发表时间: 2021-11
• 期刊: Nano Energy
• 影响因子: 17.6
• 作者: Dohyung Kim;Yongtao Liu;A. Ievlev;Kate Higgins;O. Ovchinnikova;J. Yun;J. Seidel;Sergei V. Kalinin;M. Ahmadi

Exploring the Evolution of Metal Halide Perovskites via Latent Representations of the Photoluminescent Spectra

• DOI: 10.1002/aisy.202200340
• 发表时间: 2023-01-20
• 期刊: ADVANCED INTELLIGENT SYSTEMS
• 影响因子: 7.4
• 作者: Sanchez，Sheryl;Liu，Yongtao;Ahmadi，Mahshid
• 通讯作者: Ahmadi，Mahshid

Elucidating the Spatial Dynamics of Charge Carriers in Quasi-Two-Dimensional Perovskites

• DOI: 10.1021/acsami.1c07876
• 发表时间: 2021-07-13
• 期刊: ACS APPLIED MATERIALS & INTERFACES
• 影响因子: 9.5
• 作者: Kim, Dohyung;Ahmadi, Mahshid
• 通讯作者: Ahmadi, Mahshid

Designing workflows for materials characterization

• DOI: 10.1063/5.0169961
• 发表时间: 2023-02
• 期刊: Applied Physics Reviews
• 影响因子: 15
• 作者: S. Kalinin;M. Ziatdinov;M. Ahmadi;Ayana Ghosh;Kevin M. Roccapriore;Yongtao Liu;R. Vasudevan

Understanding the ligand-assisted reprecipitation of CsPbBr3 nanocrystals via high-throughput robotic synthesis approach

• DOI: 10.1016/j.matt.2023.05.023
• 发表时间: 2023-05
• 期刊: Matter
• 影响因子: 18.9
• 作者: Sheryl L. Sanchez;Yipeng Tang;B. Hu;Jonghee Yang;M. Ahmadi