Revealing the Mechanisms of Bulk Material Dissolution in Thiol-Amine Solvent Mixtures Toward the Solution Deposition of Chalcogenide Thin Films

揭示硫醇-胺溶剂混合物中散装材料溶解对硫属化物薄膜溶液沉积的机制

• 批准号: 1904719
• 负责人: Richard Brutchey
• 金额: $ 40万
• 依托单位: University of Southern California
• 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: 2019-08-01 至 2023-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1904719&HistoricalAwards=false
• 关键词: Revealing; Mechanisms; Bulk; Material; Dissolution

NON-TECHNICAL SUMMARY: The macroelectronics industry has emerged as a powerful entity with widespread deployment of thin film technologies, such as solar cells and flat panel displays. These macroelectronics applications require innovative approaches to low-cost, large-area electronics, as the drivers are not compatible with the larger and more well-established microelectronics industry. To reduce costs and improve market potential for thin film macroelectronics, research into next-generation macroelectronic thin film deposition and processing must include a focus on low-temperature solution processing. The principal investigator is studying a solvent mixture used to dissolve cheap bulk materials to make inks that, upon solution deposition, convert to semiconductor thin films under mild conditions. The primary goals of this project include understanding the chemistry of bulk material dissolution and leveraging that information to deposit stable semiconductor thin films of novel composition that are promising for next-generation solar cells. Integrated into this plan is an outreach program specifically aimed at local community college students. The principal investigator is partnering with Cerritos Community College, an institution with a large number of underrepresented students, to provide internships on materials research. The objective of this annual 8-week outreach program is to provide these students with STEM research opportunities that are not afforded to them at the community college level, and thereby increase their transfer rate to 4-year institutions. An internship alumni network will be established to maintain formal contact with the interns after they complete the program.TECHNICAL SUMMARY: Despite decades of developments in semiconductor thin film deposition, the vast majority of methods require costly, energy intensive conditions. As such, there is a need to develop deposition processes that are less capital- and energy-intensive. The direct dissolution of bulk materials to yield solution processable inks that convert to thin films under mild conditions can result in significant cost reductions. This project directly addresses the challenge by studying inks prepared by bulk chalcogenide, oxide, and metal dissolution with thiol-amine solvent mixtures. The principal investigator is leveraging his expertise in inorganic chemistry and materials synthesis to meet the following objectives: (1) Understand the chemistry behind the dissolution of bulk materials with the thiol-amine solvent mixture. While a wide scope of bulk materials has demonstrated solubility in this solvent mixture, there is little to no understanding of the dissolution mechanism. The dissolution mechanism is being interrogated through an examination of the resulting molecular solutes and the chemical factors that affect the kinetics of dissolution. In parallel, a dual-space approach that combines Rietveld refinement and pair distribution function (PDF) analysis of X-ray total scattering data is being employed to monitor thermal conversion of the amorphous dried molecular inks into crystalline chalcogenide thin films. This approach is intelligently informing solution processing and crystallization of phase-pure, high-quality chalcogenide thin films. (2) Use the thiol-amine solvent mixture to solution process promising chalcogenide thin films for solar energy conversion. The large palette of inks now available with this system are being used to solution process more novel, compositionally complex, multinary chalcogenide semiconductor thin films with properties amenable to solar energy conversion, such as optimal band gap, polar crystal structures, and materials with high thermodynamic stability comprised of Earth abundant elements. The most promising candidates are being explored in next-generation solar cells.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.

非技术摘要：随着太阳能电池和平板显示器等薄膜技术的广泛部署，宏电子行业已经成为一个强大的实体。这些宏电子应用需要低成本、大面积电子产品的创新方法，因为驱动程序与规模更大、更成熟的微电子行业不兼容。为了降低成本和提高薄膜宏电子的市场潜力，下一代宏电子薄膜沉积和加工的研究必须包括对低温溶液加工的关注。首席研究员正在研究一种溶剂混合物，用于溶解廉价的大宗材料，以制造油墨，这些油墨在溶液沉积后，在温和的条件下转化为半导体薄膜。该项目的主要目标包括了解块状材料溶解的化学，并利用这些信息来沉积稳定的、成分新颖的半导体薄膜，这些薄膜有望用于下一代太阳能电池。该计划还纳入了一项专门针对当地社区大学生的外展计划。首席研究员正在与Cerritos社区学院合作，提供材料研究方面的实习机会。Cerritos社区学院是一所拥有大量代表不足的学生的机构。这个为期8周的年度外展计划的目标是为这些学生提供社区大学水平上无法提供的STEM研究机会，从而提高他们到四年制院校的转化率。将建立一个实习校友网络，以便在实习生完成项目后与他们保持正式联系。技术摘要：尽管半导体薄膜沉积技术已经发展了几十年，但绝大多数方法需要昂贵的、能源密集型的条件。因此，有必要开发资本和能源密集度较低的沉积过程。直接溶解大块材料以产生可溶液处理的油墨，在温和的条件下转化为薄膜，可以显著降低成本。该项目通过研究由硫化物、氧化物和金属与硫醇-胺混合溶剂溶解制备的油墨，直接解决了这一挑战。首席研究员正在利用他在无机化学和材料合成方面的专业知识来实现以下目标：(1)了解块状材料与硫醇-胺混合溶剂溶解背后的化学原理。虽然大范围的散装材料已经显示出在这种溶剂混合物中的溶解性，但对其溶解机理知之甚少甚至一无所知。正在通过对产生的分子溶质和影响溶解动力学的化学因素的检查来询问溶解机制。同时，将Rietveld精化和X射线总散射数据的对分布函数(PDF)分析相结合的双空间方法被用于监测非晶态干燥分子油墨到结晶硫化物薄膜的热转化。这一方法正在智能地指导相纯、高质量硫化物薄膜的溶液处理和结晶。(2)用硫醇-胺混合溶剂溶液制备太阳能转换用硫系化合物薄膜。该系统目前提供的大量油墨正被用于溶液加工更新颖、成分复杂的多组分硫化物半导体薄膜，这些薄膜具有适合太阳能转换的特性，如最佳带隙、极性晶体结构和由富含地球的元素组成的高热力学稳定性材料。最有希望的候选人正在探索下一代太阳能电池。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

Structural Insights on Microwave-Synthesized Antimony-Doped Germanium Nanocrystals

微波合成锑掺杂锗纳米晶体的结构见解

• DOI: 10.1021/acsnano.0c09352
• 发表时间: 2021
• 期刊: ACS Nano
• 影响因子: 17.1
• 作者: Tabatabaei, Katayoon;Sully, Heather R.;Ju, Zheng;Hellier, Kaitlin;Lu, Haipeng;Perez, Christopher J.;Newton, Kathryn A.;Brutchey, Richard L.;Bridges, Frank;Carter, Sue A.
• 通讯作者: Carter, Sue A.