CDS&E: Correlated Wavefunction Methods for Gas and Condensed Phases

普林斯顿大学的Emily Carter获得了化学理论、模型和计算方法项目的奖励，致力于开发准确、高效的从头算电子结构方法，用于预测大分子和凝聚态物质的行为。材料研究部的凝聚态物质和材料理论、计算和数据驱动材料研究项目以及计算和数据驱动科学与工程项目共同资助了该提案。Carter和他的同事们提供了解决科学和工程领域两大挑战的方法：(1)准确评估大分子的化学键离解能和反应能量；(2)准确描述凝聚态中的电荷转移和电子激发态。Carter的快速相关波函数（CW）方法在速度（利用稀缺性和并行化）和功能（通过梯度、非绝热耦合和跃迁偶极矩）方面被提升到了一个新的水平。她的基于势函数的嵌入理论结合了她的快速连续波方法，因此，例如，复杂的光激发和电极表面的电荷转移可以准确地描述。卡特和她的多学科研究小组正在开发的方法可用于预测涉及生物柴油燃料等大分子燃烧反应的大部分未开发的热化学动力学。这些基础信息对于确定如何优化可再生燃料的能源效率至关重要。该小组正在开发的其他方法将提供对燃料电池和太阳能电池的化学和物理的基本理解，并着眼于提高它们的能量转换效率。妇女和未被充分代表的少数民族参与了她的研究项目。

Emily Carter of Princeton University is supported by an award from the Chemical Theory, Models and Computational Methods Program to pursue development of accurate and efficient ab initio electronic structure methods for predicting the behavior of large molecules and condensed matter. The Condensed Matter and Materials Theory and the Computational and Data Driven Materials Research programs in the Division of Materials Research and the Computational and Data-Enabled Science and Engineering Program are co-funding this proposal. Carter and coworkers are providing the means to address two grand challenges in science and engineering: (i) accurate evaluation of chemical bond dissociation energies and reaction energetics for large molecules and (ii) accurate description of charge transfer and electronic excited states in condensed phases. Carter's fast correlated wavefunction (CW) methods are being taken to the next level in terms of speed (exploiting scarcity and via parallelization) and functionality (via gradients, nonadiabatic couplings, and transition dipole moments). Her potential-functional-based embedding theory then incorporates her fast CW methods so that, e.g., complex photo-excitation and charge transfer at electrode surfaces can be accurately described. The methods that the Carter and her multidisciplinary research group are developing can be used to predict the mostly unexplored thermochemical kinetics of combustion reactions involving very large molecules such as biodiesel fuels. This foundational information is critical to determining how to optimize the energy efficiency of renewable fuels. Other methods being developed by this group will furnish fundamental understanding of the chemistry and physics of fuel cells and solar cells, with an eye to improving their energy conversion efficiency as well. Women and under-represented minorities are involved in her research program.