Accurate Embedded-Cluster Modeling of Insulators: Applications to Metal Oxide Surface Chemistry & Surface Excitation Processes
EMSL Project ID
29790
Abstract
The accurate characterization of adsorbate reactivity and surface excitation processes at surfaces like metal oxide interfaces is key to understanding, controlling, and designing molecular interactions and transformations for new energy sources. Electronic structure of defects and localized states and surface excitation processes are two recognized challenges in catalysis and interfacial chemical sciences that defy existing levels of theory and simulation. We propose to develop a new embedded cluster model that will combine solid-state long-range effects with the highest-level electron correlated molecular theories to yield a heretofore unprecedented level of accuracy to address such problems. The new technology will leverage NWChems world-leading capabilities in coupled-cluster (CC) theory [1] (arguably the most accurate quantum chemical level of theory) with the mixed Hamiltonian methodologies to create an absolutely unique and required capability to address reactivity and excitation processes at solid-state interfaces. We will illustrate the power of the new functionality by addressing two problems of great interest to our EMSL experimental collaborators [2,3]: a) Electronic structure of defects on TiO2 surfaces; b) Surface excitation processes in NaCl.
Project Details
Start Date
2008-03-28
End Date
2010-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
: Andzelm J, BC Rinderspacher, AM Rawlett, J Dougherty, R Baer, and N Govind. 2009. "Performance of DFT Methods in the Calculation of Optical Spectra of TCF-Chromophores." Journal of Chemical Theory and Computation 5(10):2835-2846. doi:10.1021/ct900231r
Govind N, PV Sushko, WP Hess, M Valiev, and K Kowalski. 2009. "Excitons in Potassium Bromide: A Study using Embedded Time-dependent Density Functional Theory and Equation-of-Motion Coupled Cluster Methods." Chemical Physics Letters 470(4-6):353-357. doi:10.1016/j.cplett.2009.01.073
Jensen L, and N Govind. 2009. "Excited States of DNA Base Pairs Using Long-Range Corrected Time-Dependent Density Functional Theory." Journal of Physical Chemistry A 113(36):9761-9765.
Shluger AL, KP Mckenna, PV Sushko, DM Ramo, and AV Kimmel. 2009. "Modelling of electron and hole trapping in oxides." Modelling and Simulation in Materials Science and Engineering 17(084004):21. doi:10.1088/0965-0393/17/8/084004