Development and Applications of Condensed Matter Quantum Chemistry

加州大学洛杉矶分校的艾米丽·卡特得到了理论和计算化学计划和材料理论计划的支持，继续探索旨在开发系统的第一原理改进的方法，以改进密度泛函理论(DFT)对凝聚态局部区域中的能量学、结构和力的预测，使利用第一原理技术研究金属上的局部多体激发态等现象成为可能。具体的项目目标是：(1)将当前的技术扩展到多参考单双激发组态相互作用(MRSDCI)嵌入理论，以便能够定量地研究涉及多个共价键同时断裂/形成的表面反应，(2)在嵌入理论内实现缩小尺度的局部伪谱MRSDCI，以便可以研究中等分子-表面反应，(3)在嵌入理论中实施力，以便可以进行结构优化和动力学，(4)继续方法基准的各个方面，(5)将该方法应用于DFT失效的基态吸附表面体系，(6)将该方法应用于涉及多激发态的多体物理问题。发展凝聚态物质能量学、力和结构的第一原理预测的精确技术仍然是一个具有实际意义的具有挑战性的研究目标。这种计算机模拟方法的应用可以带来洞察力，鼓励将当前的技术转变为更环保的工业流程、更高效的能源和更先进的材料生产。

Emily Carter of UCLA is supported by the Theoretical and Computational Chemistry Program and the Materials Theory Program to continue exploring methodologies that aim to develop systematic first principles improvements to density functional theory (DFT) predictions of energetics, structure, and forces in a local region of condensed matter, enabling the investigation of phenomena such as local many-body excited states on metals by first principles techniques. The specific project goals are: (1) to extend the current technique to multi-reference single and double excitation configuration interaction (MRSDCI) embedding theory, in order that surface reactions involving simultaneous breaking/forming of multiple covalent bonds can be studied quantitatively, (2) to implement reduced scaling local pseudo-spectral MRSDCI within the embedding theory so that medium-sized molecule-surface reactions can be examined, (3) to implement forces in the embedding theory so that structure optimization and dynamics can be performed, (4) to continue various aspects of method benchmarking, (5) to apply the method to ground state adsorbate-surface systems where DFT has been shown to fail, (6) and to apply the method to many-body physics problems involving multiple excited states. The development of accurate techniques for the first principles prediction of condensed matter energetics, forces, and structure remains a challenging research goal with practical implications. Applications of such computer simulation methods can lead to insights that encourage changes in current technologies to more environmentally friendly industrial processes, more efficient sources of energy, and the production of more advanced materials.