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.
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.
