GOALI: Structural and Topological Controls on Viscoelasticity and Relaxation Processes in Chalcogenide Glass-Forming Liquids

目标：硫族化物玻璃形成液体中粘弹性和弛豫过程的结构和拓扑控制

• 批准号: 1855176
• 负责人: Sabyasachi Sen
• 金额: $ 77.12万
• 依托单位: University of California-Davis
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-05-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1855176&HistoricalAwards=false
• 关键词: GOALI; Structural; Topological; Controls; Viscoelasticity

NON-TECHNICAL DESCRIPTION: Chalcogenide (non-oxide alloys or compounds containing sulfur, selenium or tellurium) glasses are an important class of materials with wide-ranging applications in the areas of photonics, telecommunication, memory storage, photovoltaics and environmental remote sensing. A fundamental understanding of the dynamical processes associated with the temperature- and composition- dependent flow behavior of the parent melts or liquids from which these glasses are derived, is crucial in all stages of their industrial production. This project aims to provide unique knowledge regarding the connection between the "microscopic (atomistic)" and the "macroscopic" aspects of the dynamical behavior of chalcogenide liquids for the very first time, using a combination of cutting-edge characterization techniques. This knowledge is key to the optimization of the chemistry and processing parameters of these materials for improved and novel functionality, thereby enabling their application in modern transformative technologies with strong societal impact. Scientifically, this work impacts materials science, physical chemistry, and solid-state physics. The interdisciplinary nature of this work transfers knowledge between fields and provides students with unique opportunities for intellectual growth. Graduates typically find employment in both academia and in glass and semiconductor industry. The impact of this project in terms of education and outreach is in three major areas: (1) participation by students in research, (2) active and tight-knit collaboration with industry (Corning, Inc.) where students are mentored and gain understanding of industry priorities, and (3) dissemination of knowledge about glass science and technology to the broader scientific community. The research findings are embedded into special topics courses that are offered to students in materials science, chemistry, and other related fields; and they contribute to campus programs for women and minority students and to the recruitment of promising students from underrepresented and economically-disadvantaged groups.TECHNICAL DETAILS: The dynamical processes in supercooled glass-forming liquids, associated with their viscous flow, structural relaxation and annealing near the glass transition, control all aspects of the processing and technological utility of the resulting glasses and glass-ceramics. However, surprisingly enough, little is known regarding the connection between the atomic structure, its connectivity and topology and the temperature dependence of the flow behavior of chalcogenide liquids. Historically, therefore, much of the approach for designing new chalcogenide glasses has been largely empirical and lacked the predictive power needed for their compositional optimization and processing methods. This GOALI project brings together investigators with complementary expertise and common interests from UC Davis (Sen, PI) and from Corning Incorporated (Aitken, co-PI), to investigate the effects of structural connectivity and topology on the temperature dependence of the viscoelastic behavior and relaxation processes in supercooled chalcogenide (sulfide and selenide) liquids, using a unique combination of state-of-the-art oscillatory parallel-plate rheometry, dynamical nuclear magnetic resonance (NMR) spectroscopy and differential scanning calorimetry measurements. Predictive atomistic models of structure-relaxation-viscous flow relationships, built on the basis of the results obtained in this project, may enable the optimization of the chemistry, synthesis, and processing parameters of these complex materials for a wide range of modern technological applications. The focus of this project, namely how and why, the various aspects of the atomic structure control the temperature dependent viscoelasticity, relaxational behavior and related phenomena in chalcogenide glass-forming liquids is in itself crosscutting materials research. The breadth, flexibility and interdisciplinary nature of this project prepare the students with powerful experimental skills and research experience in both academic and industrial settings that may open many future career opportunities. It also enriches the graduate education and training experience through numerous scientific interactions between the collaborating scientists and participating students.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.

非技术描述：硫系(含硫、硒或碲的非氧化物合金或化合物)玻璃是一类重要的材料，在光子学、电信、存储、光伏和环境遥感等领域有着广泛的应用。对这些玻璃的母体熔体或液体与温度和成分相关的流动行为的动力学过程的基本了解，在它们的工业生产的所有阶段都是至关重要的。该项目旨在利用尖端表征技术的组合，首次提供有关硫化物液体动力学行为的“微观(原子)”和“宏观”方面之间的联系的独特知识。这些知识对于优化这些材料的化学和工艺参数以实现改进和新颖的功能至关重要，从而使它们能够应用于具有强大社会影响的现代变革性技术。从科学上讲，这项工作影响到材料科学、物理化学和固体物理学。这项工作的跨学科性质在不同领域之间传递知识，并为学生提供独特的智力增长机会。毕业生通常在学术界以及玻璃和半导体行业找到工作。该项目在教育和外展方面的影响主要体现在三个方面：(1)学生参与研究，(2)与工业界积极而紧密的合作(康宁公司)指导学生并了解行业优先事项，以及(3)向更广泛的科学界传播有关玻璃科学和技术的知识。这些研究成果被嵌入到为材料科学、化学和其他相关领域的学生提供的专题课程中；它们有助于为女性和少数族裔学生提供校园项目，并有助于从代表不足和经济困难群体中招收有前途的学生。技术细节：过冷玻璃形成液体中的动态过程，与它们在玻璃转变附近的粘性流动、结构松弛和退火有关，控制着所产生的玻璃和微晶玻璃的加工和技术实用的方方面面。然而，令人惊讶的是，关于原子结构、它的连接性和拓扑与硫化物液体流动行为的温度相关性之间的联系，人们知之甚少。因此，从历史上看，设计新的硫系玻璃的方法大多是经验的，缺乏成分优化和加工方法所需的预测能力。这个GOALI项目汇集了来自加州大学戴维斯分校(Sen，PI)和康宁公司(Aitken，co-PI)的具有互补专业知识和共同兴趣的研究人员，使用最先进的振荡平行板流变仪、动态核磁共振(NMR)谱和差示扫描量热仪测量的独特组合，研究了结构连通性和拓扑对过冷硫化物(硫化物和硒)液体中粘弹性行为和松弛过程的温度依赖性的影响。根据本项目所获得的结果建立的结构-松弛-粘性流动关系的预测原子学模型，可能使这些复合材料的化学、合成和工艺参数优化，以用于广泛的现代技术应用。这个项目的重点，即原子结构的各个方面如何以及为什么控制硫化物玻璃形成液中随温度变化的粘弹性、松弛行为和相关现象，本身就是交叉材料研究。这个项目的广度、灵活性和跨学科性质使学生在学术和工业环境中拥有强大的实验技能和研究经验，这可能会为未来的职业机会提供机会。它还通过合作的科学家和参与的学生之间的大量科学互动，丰富了研究生教育和培训经验。该奖项反映了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

Observation of a reentrant structural transition in an arsenic sulfide liquid

硫化砷液体中重入结构转变的观察

• DOI: 10.1063/5.0107799
• 发表时间: 2022
• 期刊: The Journal of Chemical Physics
• 作者: Yuan, Bing;Aitken, Bruce G.;Sen, Sabyasachi
• 通讯作者: Sen, Sabyasachi

Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition

• DOI: 10.1038/s41598-020-62783-5
• 发表时间: 2020-04
• 期刊: Scientific Reports
• 影响因子: 4.6
• 作者: Jianheng Li;R. Jangid;Weidi Zhu;Chris Kohne;A. Fluerasu;Yugang Zhang;S. Sen;R. Kukreja

Aging-Induced Structural Evolution of a GeSe 2 Glass Network: The Role of Homopolar Bonds

GeSe 2 玻璃网络的老化引起的结构演化：同极性键的作用

• DOI: 10.1021/acs.jpcb.1c08836
• 发表时间: 2022
• 期刊: The Journal of Physical Chemistry B
• 作者: Yuan, Bing;Chen, Hao;Sen, Sabyasachi
• 通讯作者: Sen, Sabyasachi

Structure and Fragility of Zn-phosphate glasses: Results from multinuclear NMR spectroscopy and calorimetry

• DOI: 10.1016/j.jnoncrysol.2022.121395
• 发表时间: 2022-03
• 期刊: Journal of Non-Crystalline Solids
• 影响因子: 3.5
• 作者: Yiqing Xia;Hao Chen;I. Hung;Z. Gan;S. Sen

Rheology of supercooled Se-Te chain liquids: Role of Te as an interchain cross-linker

过冷 Se-Te 链液体的流变学：Te 作为链间交联剂的作用

• DOI: 10.1016/j.jnoncrysol.2019.119764
• 发表时间: 2020
• 期刊: Journal of Non-Crystalline Solids
• 影响因子: 3.5
• 作者: Yuan, Bing;Aitken, Bruce;Sen, Sabyasachi
• 通讯作者: Sen, Sabyasachi