Conversion Processing of Functional Oxides to Oxyfluorides

功能性氧化物向氟氧化物的转化处理

• 批准号: 1562223
• 负责人: Steven May
• 金额: $ 29.97万
• 依托单位: Drexel University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-07-01 至 2020-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1562223&HistoricalAwards=false
• 关键词: Conversion; Processing; Functional; Oxides; Oxyfluorides

Complex oxides play a critical role in wide-ranging technologies that underpin modern society with applications in the energy, communications, and health sectors. The ability to make thin films of these materials will enable new applications in electronics and energy conversion. However, in order to fully harness the potential of oxide films, new processing approaches are required that will enable a wider range of material compositions to be manufactured. This award supports fundamental research focused on developing and understanding strategies for the controlled substitution of fluorine for oxygen, thereby enabling new means to engineer electronic, optical, and magnetic properties of thin films and nanomaterials. The processing methods to be studied are scalable, require minimal capital investment, and can be carried out on a broad range of oxide films, independent of how the materials were first processed. As such, the research will directly support the nation's strategic goal of developing agile new approaches for materials processing that can reduce the time from material discovery to technological deployment. The research will also benefit the U.S. economy by contributing to the advanced engineering education of the participating students. While advances in deposition techniques have enabled the processing of perovskite oxide films with monolayer precision, expanding access to new material chemistries remains a challenge. This project is focused on the substitution of fluorine for oxygen, which allows for control of the transition metal cation valence state and the covalency of the metalanion bond, both effects having profound implications for electronic, ferroic, and optical properties. This research will elucidate fundamental scientific mechanisms in the synthesis of oxyfluoride mixed-anion perovskites based on post-growth conversion reactions of oxide films. The conversion processes to be studied utilize vapor transport and anion diffusion from fluoropolymers. The team will deposit oxide films, carry out fluorination reactions, and utilize spectroscopic and structural characterization techniques to develop a predictive understanding of how the resultant anion composition can be engineered through processing conditions to tune functional properties.

复杂氧化物在支撑现代社会的广泛技术中发挥着关键作用，这些技术在能源、通信和卫生领域都有应用。利用这些材料制造薄膜的能力将使电子和能源转换领域的新应用成为可能。然而，为了充分利用氧化膜的潜力，需要新的加工方法来制造更广泛的材料成分。该奖项支持基础研究，重点是开发和理解氟对氧的受控替代策略，从而实现设计薄膜和纳米材料的电子、光学和磁性特性的新方法。所研究的加工方法具有可扩展性，需要最少的资本投资，并且可以在广泛的氧化膜上进行，而与材料的首次加工方式无关。因此，该研究将直接支持国家开发敏捷的材料加工新方法的战略目标，该方法可以缩短从材料发现到技术部署的时间。该研究还将通过促进参与学生的高级工程教育而造福美国经济。虽然沉积技术的进步已经能够以单层精度加工钙钛矿氧化物薄膜，但扩大新材料化学的使用仍然是一个挑战。该项目的重点是用氟取代氧，从而可以控制过渡金属阳离子价态和金属阴离子键的共价性，这两种效应对电子、铁性和光学性质都有深远的影响。这项研究将阐明基于氧化膜生长后转化反应合成氟氧化物混合阴离子钙钛矿的基本科学机制。要研究的转化过程利用含氟聚合物的蒸气传输和阴离子扩散。该团队将沉积氧化物薄膜，进行氟化反应，并利用光谱和结构表征技术来预测如何通过加工条件设计所得阴离子组合物以调整功能特性。

项目成果

Synthesis and Characterization of SrFe x Mn 1–x (O,F) 3−δ Oxide (δ = 0 and 0.5) and Oxyfluoride Perovskite Films

SrFe x Mn 1âx (O,F) 3âδ 氧化物（δ = 0 和 0.5）和氟氧化钙钛矿薄膜的合成和表征

• DOI: 10.1021/acs.inorgchem.0c01148
• 发表时间: 2020
• 期刊: Inorganic Chemistry
• 影响因子: 4.6
• 作者: Wang, Jiayi;Lefler, Benjamin M.;May, Steven J.
• 通讯作者: May, Steven J.

Physical properties of epitaxial SrMnO 2.5−δ F γ oxyfluoride films

外延SrMnO 2.5-δ F γ氟氧化物薄膜的物理性能

• DOI: 10.1088/1361-648x/ab2414
• 发表时间: 2019
• 期刊: Journal of Physics: Condensed Matter
• 作者: Wang, Jiayi;Shin, Yongjin;Gauquelin, Nicolas;Yang, Yizhou;Lee, Christopher;Jannis, Daen;Verbeeck, Johan;Rondinelli, James M;May, Steven J
• 通讯作者: May, Steven J

Reconfigurable lateral anionic heterostructures in oxide thin films via lithographically defined topochemistry

• DOI: 10.1103/physrevmaterials.3.073802
• 发表时间: 2019-07-08
• 期刊: PHYSICAL REVIEW MATERIALS
• 影响因子: 3.4
• 作者: Lefler, Benjamin M.;Duchon, Tomas;May, Steven J.
• 通讯作者: May, Steven J.

Role of fluoride and fluorocarbons in enhanced stability and performance of halide perovskites for photovoltaics

• DOI: 10.1103/physrevmaterials.4.120301
• 发表时间: 2020-12
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: Benjamin M. Lefler;S. May;A. Fafarman

Strain-Induced Anion-Site Occupancy in Perovskite Oxyfluoride Films

• DOI: 10.1021/acs.chemmater.0c04793
• 发表时间: 2021-02
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Jiayi Wang;Yongjin Shin;J. Paudel;J. Grassi;R. Sah;Weibing Yang;E. Karapetrova;A. Zaidan;V. Strocov;C. Klewe;P. Shafer;A. Gray;J. Rondinelli;S. May