DMREF/Collaborative Research: Chemoresponsive Liquid Crystals Based on Metal Ion-Ligand Coordination

DMREF：合作研究：基于金属离子-配体配位的化学反应液晶非技术描述：基于计算机的方法可以预测材料性能，有可能将当前的材料设计范式转变为基于计算、实验和数据分析的集成“周期”，从而大大加速材料的开发，同时降低成本。DMREF项目旨在通过组建一个跨学科团队来推进这一愿景，该团队在计算化学（Mavrikakis）、合成有机化学（Twieg）和物理性质测量（Abbott）方面具有深刻的见解。该团队将解决加速部署基于液晶（lc）的有前途的化学反应材料的挑战。除了解决与化学功能化LCs和界面设计相关的基本科学问题外，该项目还将推进这些材料的巨大技术和社会潜力，作为新型传感器和执行器的基础，例如，可用于气候变化的环境监测、有毒工业化学品或化学战剂的检测。测量呼吸中的挥发性气体作为疾病的指标。该DMREF项目创造的多学科环境也将有助于培养完全精通新材料部署范例的下一代劳动力，该范例集成了计算化学，合成和性能表征，以快速设计和实现功能材料。调查人员将利用该项目开发新的大学水平的教育材料，以及新的公共宣传工作和参与代表性不足群体的计划。这个DMREF团队的成员都有创业的记录；参与该项目的学生和博士后将有机会参与创业活动。该小组的所有努力将通过一种数据管理方法进行整合，该方法还旨在与美国主要国家数据库进行接口，从而通过为更广泛的科学和工业界提供不受限制的数据和元数据访问，为材料基因组计划的国家基础设施做出贡献。技术描述：在过去的十年中，艰苦而缓慢的实验努力已经证明了化学反应液晶（lc）在传感一类重要化学靶标（有机膦酸盐）方面的前景。然而，这些原理要普遍得多，因此有机会设计出化学上量身定制的lc和界面，以选择性地响应许多其他类型的目标分子。该DMREF项目将通过整合计算周期（在几个级别上执行，称为世代）、新型介原的有机合成和物理性质评估来解决这一广泛的机会，以加快LC材料的设计时间，这些材料可以选择性地响应社会重要的化学物质，如HCN、（CH3）2CO、HCHO、O3、CO、NH3、NO、ClCN、CO2、NO2和H2O。这个DMREF项目的智力价值的一个关键方面在于新知识的发展，这将使计算，实验和数据分析的集成功能材料的设计。计算（在电子结构水平上）、功能介原的合成和性质表征之间的密切反馈将导致每种方法的进步，这将为基于金属配体配位的化学反应液晶材料的设计定义新的原则。它还将为我们理解化学反应材料的分层设计、软物质的界面有序以及使用金属离子-配体配位相互作用来控制lc的界面有序提供基础进展。

DMREF: Collaborative Research: Chemoresponsive Liquid Crystals Based on Metal Ion-Ligand CoordinationNon-Technical Description: Computer-based methods that can predict materials properties have the potential to transform the current materials design paradigm into one based on integrated "cycles" of computation, experimentation and data analysis, thereby substantially accelerating materials development while decreasing costs. This DMREF project seeks to advance this vision through the formation of an interdisciplinary team with deep insight in computational chemistry (Mavrikakis), synthetic organic chemistry (Twieg) and physical property measurement (Abbott). The team will tackle the challenge of accelerating deployment of promising classes of chemically-responsive materials that are based on liquid crystals (LCs). In addition to addressing fundamental scientific questions related to the design of chemically functionalized LCs and interfaces, the project will advance the enormous technological and societal potential of these materials as the basis of new classes of sensors and actuators that can, for example, be used in the context of environmental monitoring of climate change, detection of toxic industrial chemicals or chemical warfare agents, and measurement of volatile gases in breath as an indicator of disease. The multi-disciplinary environment created by this DMREF project will also contribute to the training of a next generation workforce fully versed in the new materials deployment paradigm that integrates computational chemistry, synthesis and property characterization to rapidly design and realize functional materials. The project will be leveraged by the investigators to develop new university-level educational materials as well as new programs for public outreach efforts and engagement of underrepresented groups. Members of this DMREF team have a record of entrepreneurism; students and postdoctoral fellows engaged in this project will be provided with opportunities to participate in entrepreneurial activities. All of the efforts of the group will be integrated by an approach to data management that is designed also to interface to key US national databases and thus contribute to the Materials Genome Initiative national infrastructure by providing unfettered access to data and metadata for the broader scientific and industrial community. Technical Description: Laborious and slow experimental efforts over the past decade have demonstrated the promise of chemoresponsive liquid crystals (LCs) in the context of sensing one important class of chemical targets (organophosphonates). The principles, however, are far more general and thus an opportunity exists to design chemically tailored LCs and interfaces that respond selectively to many other classes of target molecules. This DMREF project will address this broad opportunity by integrating cycles of computation (performed at several levels, called Generations), organic synthesis of novel mesogens and physical property evaluation to accelerate the timeline for design of LC materials that respond selectively to societally important chemical species such as HCN, (CH3)2CO, HCHO, O3, CO, NH3, NO, ClCN, CO2, NO2 and H2O. A key aspect of the intellectual merit of this DMREF project lies in the development of new knowledge that will enable integration of computation, experiment and data analysis for the design of functional materials. The close feedback between computation (at the level of electronic structure), synthesis of functional mesogens and property characterization, which will lead to advances in each methodology, will define new principles for the design of chemoresponsive liquid crystalline materials based on metal-ligand coordination. It will also provide fundamental advances in our understanding of hierarchical design of chemically responsive materials, interfacial ordering of soft matter, and the use of metal ion-ligand coordination interactions to control the interfacial ordering of LCs.