CAREER: Exploiting Open-Shell Character for Organic Optoelectronic Applications

职业：利用开壳特性进行有机光电应用

• 批准号: 2045920
• 负责人: Mark Chen
• 金额: $ 54.91万
• 依托单位: Lehigh University
• 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: 2021-05-01 至 2026-04-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2045920&HistoricalAwards=false
• 关键词: CAREER; Exploiting; Open; Shell; Character

With support from the Chemical Structure, Dynamics, and Mechanisms B Program in the Division of Chemistry and the Electronic and Photonic Materials Program in the Division of Materials Science, Dr. Mark Chen at Lehigh University will develop new carbon-based materials that exploit properties of novel molecular radicals which have unpaired electron character. Most organic molecules only contain spin-paired electrons. This ensures environmental stability but limits the capabilities of molecular materials for optoelectronic applications. In this project, Dr. Chen and his students are using rational design principles to construct new molecular radicals that are expected to have high environmental stability, ultimately leading to enhanced device performance when employed as luminescent and charge transport materials. The project involves a combination of chemical synthesis, followed by physical characterization studies to identify and optimize molecular structures and properties. This interdisciplinary research facilitates the development of educational course materials, which are designed to inspire science, technology, engineering and mathematics (STEM) students to think outside the boundaries of formal disciplines. Interconnections within STEM will be promoted through outreach events aimed at recruiting student groups from the mid-Atlantic region who are underrepresented in STEM fields. Research activities in this project are aimed at the development of new electronic materials which can exploit the effects of open-shell electronic structure. For stability, most organic molecules possess closed-shell electronic structures, where all electrons within a molecule are spin-paired. This inherently limits optoelectronic applications due to unfavorable energies related to emission mechanisms and charge transfer kinetics. In this project, Professor Chen and his students will synthesize and systematically explore the structure-property relationships of air-stable, pi-conjugated molecules with bisphenalenyl structures that possess persistent unpaired spin. This research builds on an efficient synthetic route already developed by the Chen research group. Synthetic modifications of bisphenalenyl structures are designed to control emission wavelength and quantum efficiencies during luminescence, while also enhancing electron mobilities and conductivities during charge transport. Research in this project is expected to impact society by introducing new optoelectronic materials and devices that are more portable, energy efficient, and less expensive to manufacture. This interdisciplinary research, which relies on chemical synthesis and diverse methods of physical characterization, provides diverse professional training opportunities for graduate and undergraduate students. New curricula and outreach programs will inspire students to cultivate broader interests in STEM careers.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.

在化学系化学结构、动力学和机理 B 项目以及材料科学系电子和光子材料项目的支持下，理海大学的 Mark Chen 博士将开发新型碳基材料，该材料利用具有不成对电子特征的新型分子自由基。大多数有机分子仅含有自旋配对电子。 这确保了环境稳定性，但限制了分子材料用于光电应用的能力。在这个项目中，陈博士和他的学生正在利用合理的设计原理来构建新的分子自由基，这些分子自由基预计具有较高的环境稳定性，最终在用作发光和电荷传输材料时提高器件性能。该项目涉及化学合成和物理表征研究的结合，以识别和优化分子结构和特性。这种跨学科研究促进了教育课程材料的开发，这些材料旨在激发科学、技术、工程和数学 (STEM) 学生在正式学科的界限之外进行思考。将通过旨在招募来自大西洋中部地区 STEM 领域代表性不足的学生团体的外展活动来促进 STEM 内部的相互联系。该项目的研究活动旨在开发能够利用开壳电子结构效应的新型电子材料。 为了稳定性，大多数有机分子具有闭壳电子结构，其中分子内的所有电子都是自旋配对的。由于与发射机制和电荷转移动力学相关的不利能量，这本质上限制了光电应用。 在这个项目中，陈教授和他的学生将合成并系统地探索具有持久不成对自旋的双酚基结构的空气稳定的π共轭分子的结构-性质关系。这项研究建立在陈研究小组已经开发的高效合成路线的基础上。双酚基结构的合成修饰旨在控制发光过程中的发射波长和量子效率，同时还增强电荷传输过程中的电子迁移率和电导率。该项目的研究预计将通过引入更便携、更节能且制造成本更低的新型光电材料和设备来影响社会。这种依赖化学合成和多种物理表征方法的跨学科研究，为研究生和本科生提供了多样化的专业培训机会。新课程和推广计划将激励学生在 STEM 职业中培养更广泛的兴趣。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

Chemically Triggered Release of Singlet Oxygen from Bisphenalenyl Endoperoxides with a Brønsted Acid

用布伦斯台德酸化学触发双酚基内过氧化物释放单线态氧

• DOI: 10.1021/acs.orglett.2c00340
• 发表时间: 2022-03
• 期刊: Organic Letters
• 影响因子: 5.2
• 作者: Imran, Muhammad;Chen, Mark S.
• 通讯作者: Chen, Mark S.

Self-Sensitized and Reversible O 2 Reactivity with Bisphenalenyls for Simple, Tunable, and Multicycle Colorimetric Oxygen-Sensing Films

与双酚基的自敏和可逆 O 2 反应性，用于简单、可调和多循环比色氧传感薄膜

• DOI: 10.1021/acsami.1c16033
• 发表时间: 2022-01
• 期刊: ACS Applied Materials & Interfaces
• 影响因子: 9.5
• 作者: Imran, Muhammad;Chen, Mark S.
• 通讯作者: Chen, Mark S.