Development and Applications of Condensed Matter Quantum Chemistry

Princeton University, Princeton NJ

Investigators

Abstract

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.