CAREER: Developing Wavefunction-based Quantum Chemistry for Solids

在化学系化学理论、模型和计算方法计划和已建立的促进竞争研究计划(EPSCoR)的支持下，爱荷华大学的詹姆斯·谢泼德博士将开发用于预测固体整体性质的高精度基态波函数电子结构方法。新型量子材料由于其电子结构的特殊性而具有独特的性质，因此有可能推动技术变革。这些材料的例子包括催化剂和半导体。当计算化学家能够忠实地为这些化合物的电子结构建模时，他们可以与实验者一起为材料的合理设计做出贡献。谢泼德研究小组正在寻求能够更快、更准确地进行此类计算的工具。这些工具有望促进我们对电子在固体中如何相互作用的理论理解。谢泼德研究小组还在开发一项基于课程的本科生研究计划，采用基于证据的设计理念。该项目将培训STEM(科学、技术、工程和数学)专业的本科生，学习新材料的计算机辅助设计，以适应学术界和工业界对计算指导材料设计兴趣的上升。此外，该计划将寻求提高STEM专业学生的留存率，特别是那些来自代表性不足群体的学生。在这个项目中，爱荷华大学的詹姆斯·谢泼德博士和他的研究小组正在努力改进高精度计算化学方法，如耦合团簇理论和全组态相互作用量子蒙特卡罗。这些方法的广泛采用受到了有限大小误差的阻碍，这些误差是由于试图模拟具有有限原子数量的真实系统而产生的。谢泼德研究小组正在系统地研究这些错误的物理根源；为基于波函数的量子化学消除这些错误；并利用这些技术来研究催化剂和半导体设计。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。

With support from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry, and the Established Program to Stimulate Competitive Research (EPSCoR) Dr. James Shepherd of the University of Iowa will be developing high-accuracy ground-state wavefunction electronic structure methods for the prediction of bulk properties of solids. Novel quantum materials have the potential to drive technological change due to the unique properties they possess as a result of the specific nature of their electronic structure. Examples of these materials include catalysts and semiconductors. When computational chemists are able to faithfully model the electronic structure of these compounds, they can contribute to the rational design of materials alongside experimentalists. The Shepherd research group is pursuing tools that enable quicker and more accurate such calculations. These tools are expected to advance our theoretical understanding of how electrons interact in solids. The Shepherd research group is also developing a course-based undergraduate research program using an evidence-based design philosophy. This program will train undergraduate STEM (Science, Technology, Engineering and Mathematics) majors in the computer-aided design of new materials commensurate with the uptick in interest in computationally guided materials design in academia and industry. Additionally, the program will seek to improve retention of students in STEM majors, especially of those students from underrepresented groups.In this project, Dr. James Shepherd and his research group at the University of Iowa are working to improve high accuracy computational chemistry methods, such as coupled cluster theory and full configuration interaction quantum Monte Carlo. The widespread adoption of these methods is prevented by finite size errors, which arise from trying to simulate real systems with a limited number of atoms. The Shepherd research group is systematically studying the physical origin of these errors; removing these errors for wavefunction-based quantum chemistry; and leveraging these technologies to study catalyst and semiconductor design.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.