Collaborative Proposal: Multidimensional Tracking of Local Environment-Affected Transport Pathways in Perovskite Solar Cells

合作提案：钙钛矿太阳能电池中受局部环境影响的传输路径的多维跟踪

• 批准号: 1906029
• 负责人: Sean Shaheen
• 金额: $ 26.99万
• 依托单位: University of Colorado at Boulder
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1906029&HistoricalAwards=false
• 关键词: Collaborative; Proposal; Multidimensional; Tracking; Local

Organic metal halide perovskites have gained enormous research interest as materials for solar cells, and their efficiencies are now approaching those of conventional silicon devices. Additionally, they allow for more scalable fabrication and for the development of higher efficiency tandem devices with two different absorbers. Perovskites have a complicated crystal structure with many forms of disorder. Despite this complexity, they have a robust ability to transport charges without losses that reduce efficiency. However, fundamental questions regarding the role of the disorder and its effect on the generated photocurrent remain unanswered. This project uses advanced, ultrafast spectroscopy to measure the effects of disorder on energy and charge carrier flow in perovskites. These results are directly coupled to the subsequent device behavior. Overall, this project provides an understanding of the fundamental physics of the materials while also providing guidance on practical methods to improving device efficiencies. The principal investigators will use this research topic to engage with K-12 students, undergraduate students, and community college teachers in research. They will also reach out to the general public through public lectures, hands-on presentations at a local amusement park, and online classes.The objective of the project is to measure the effect of spatial irregularity from defects and mobile cations on exciton and free carrier transport in perovskite thin-film photovoltaic materials and devices. Multidimensional coherent spectroscopy experiments will be performed in a tight feedback loop with controlled and scalable synthesis enabling new understanding of microscopic carrier transport to spark transformative gains in device efficiency. Experiments are performed on perovskite materials and photovoltaic devices in order to: 1.) quantify the effect of defect density on carrier transport and dynamics through a novel implementation of multidimensional coherent spectroscopy; 2.) measure the effect of both static and dynamic cation disorder on carrier lifetime; 3.) optimize material composition and device architecture through close coupling between optical experiments and device fabrication; and 4.) characterize scalable deposition techniques and their effect on film heterogeneity at varying size scales. As part of the work, new experimental approaches are developed, including a) simultaneous detection of photoluminescence and photocurrent through multidimensional spectroscopy and b) energy-coupled deposition of the perovskite materials to yield improved film quality for scalable device fabrication.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.

有机金属卤化物钙钛矿作为太阳能电池材料引起了巨大的研究兴趣，其效率现已接近传统硅器件的效率。此外，它们还允许更可扩展的制造以及开发具有两种不同吸收器的更高效率的串联装置。钙钛矿具有复杂的晶体结构，具有多种无序形式。尽管存在这种复杂性，但它们具有强大的传输电荷的能力，而不会造成效率降低的损失。然而，关于这种无序的作用及其对产生的光电流的影响的基本问题仍未得到解答。该项目使用先进的超快光谱来测量钙钛矿中无序对能量和电荷载流子流的影响。这些结果直接耦合到后续的设备行为。总体而言，该项目提供了对材料的基本物理原理的理解，同时还为提高设备效率的实用方法提供了指导。主要研究人员将利用该研究课题与 K-12 学生、本科生和社区学院教师进行研究。他们还将通过公开讲座、当地游乐园的实践演示和在线课程来接触公众。该项目的目标是测量缺陷和移动阳离子造成的空间不规则性对激子和自由载流子的影响钙钛矿薄膜光伏材料和器件中的传输。多维相干光谱实验将在紧密的反馈环路中进行，并通过受控和可扩展的合成来实现对微观载流子传输的新理解，从而激发器件效率的变革性收益。在钙钛矿材料和光伏器件上进行实验，目的是：1）通过多维相干光谱的新颖实现来量化缺陷密度对载流子传输和动力学的影响； 2.) 测量静态和动态阳离子无序对载流子寿命的影响； 3.) 通过光学实验和器件制造之间的紧密耦合来优化材料成分和器件结构； 4.) 表征可扩展的沉积技术及其对不同尺寸尺度的薄膜异质性的影响。作为工作的一部分，开发了新的实验方法，包括 a) 通过多维光谱同时检测光致发光和光电流，b) 钙钛矿材料的能量耦合沉积，以提高薄膜质量，用于可扩展的设备制造。该奖项反映了 NSF 的法定使命，并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，被认为值得支持。

项目成果

Lateral spectrum splitting system with perovskite photovoltaic cells

钙钛矿光伏电池横向光谱分裂系统

• DOI: 10.1117/1.jpe.12.022206
• 发表时间: 2022-04-01
• 期刊: Journal of Photonics for Energy
• 影响因子: 1.7
• 作者: Benjamin D. Chrysler;S. Shaheen;R. Kostuk
• 通讯作者: R. Kostuk

Ultrafast nano-imaging of polaron dynamics in lead halide perovskites

卤化铅钙钛矿中极化子动力学的超快纳米成像

• DOI: 10.1364/up.2020.m3a.8
• 发表时间: 2020-10
• 期刊: The 22nd International Conference on Ultrafast Phenomena 2020
• 作者: Nishida, Jun;Chang, Peter T.;Ye, Jiselle;Shaheen, Sean E.;Raschke, Markus B.
• 通讯作者: Raschke, Markus B.

Nanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites

三重阳离子钙钛矿中超快多体载流子动力学的纳米级异质性

• DOI: 10.1038/s41467-022-33935-0
• 发表时间: 2022-11-03
• 期刊: Nature Communications
• 影响因子: 16.6
• 作者: J. Nishida;Peter T. S. Chang;Jiselle Y. Ye;Prachi Sharma;Dylan M. Wharton;Samuel C. Johnson;S. Shahe
• 通讯作者: S. Shahe

Ultrafast Heterodyne Infrared Nano-Imaging of Polaron Dynamics in Lead Halide Perovskites

卤化铅钙钛矿中极化子动力学的超快外差红外纳米成像

• DOI: 10.1364/cleo_qels.2021.ftu4i.5
• 发表时间: 2021-10
• 期刊: Quantum Electronics and Laser Science
• 作者: Nishida, J;Ye, J;Sharma, P;Shaheen, S. E.;Raschke, M. B.
• 通讯作者: Raschke, M. B.

Heterogeneous Cation–Lattice Interaction and Dynamics in Triple-Cation Perovskites Revealed by Infrared Vibrational Nanoscopy

红外振动纳米显微镜揭示三阳离子钙钛矿中的异质阳离子—晶格相互作用和动力学

• DOI: 10.1021/acsenergylett.0c00522
• 发表时间: 2020-05
• 期刊: ACS Energy Letters
• 影响因子: 22
• 作者: Nishida, Jun;Alfaifi, Amani H.;Gray, Thomas P.;Shaheen, Sean E.;Raschke, Markus B.
• 通讯作者: Raschke, Markus B.