Development and Applications of Condensed Matter Quantum Chemistry

加州大学洛杉矶分校的Emily Carter在理论与计算化学项目和材料理论项目的支持下，继续探索方法，旨在发展系统的第一性原理，改进密度泛函数理论（DFT）对凝聚态局部区域的能量学、结构和力的预测，从而通过第一性原理技术研究金属的局部多体激发态等现象。具体的项目目标是：(1)将现有技术扩展到多参考单激发和双激发构型相互作用（MRSDCI）嵌入理论，以便定量研究涉及多个共价键同时断裂/形成的表面反应；(2)在嵌入理论中实现局部伪谱MRSDCI的降标度，以便研究中型分子-表面反应；(3)在嵌入理论中实施力，以便进行结构优化和动力学，(4)继续进行方法基准测试的各个方面，(5)将该方法应用于DFT已被证明失效的基态吸附表面系统，(6)并将该方法应用于涉及多个激发态的多体物理问题。发展精确的技术来预测凝聚态物质的能量、力和结构，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深刻的见解，鼓励当前技术向更环保的工业过程、更有效的能源和更先进材料的生产转变。

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.