Use FLO-SIC to eliminate self-interaction error.
Refine the algorithmic steps in the FLO-SIC method and optimize the FLO-SIC software.
Synthesize improved molecular magnet compounds, guided by FLO-SIC calculations.
Synthesize and characterize MOF-based catalysts, guided by FLO-SIC calculations.
Use FLOSIC to eliminate self-interaction error from the most sophisticated DFT methods to improve the accuracy and reliability of materials calculations. The theory effort can be divided into two parts. The first involves merging the FLOSIC methodology with the most sophisticated – and successful - semi-local density functionals. The object is to devise an effective way to correct self-interaction errors where needed, without degrading the performance of the functionals where they already work well. The second theory initiative is investigating how to use results from FLOSIC calculations to eliminate self-interaction effects from time-dependent density functional theory calculations.
Many-body electron theory, density functional theory, computational materials science
Density-functional theory, materials theory, quantum chemistry
Refine the algorithmic steps in the FLO-SIC method and optimize the FLOSIC software to enable efficient, self-interaction-free calculations. The Code and Method Development research is aimed at creating improved algorithms and software for implementing FLOSIC efficiently in electronic structure calculations. The coding effort includes achieving highly parallelized software that will take advantage of next generation high performance computers. Method development objectives include instituting periodic boundary conditions and relativity to enable calculations on materials containing atoms from across the periodic table. These groups will also provide support to the Theory Thrust by critically assessing the success of FLOSIC for eliminating self-interaction errors in practice.
Properties of large, fullerene-like clusters, scientific programming for electronic structure methods
Light-harvesting in nanostructures, molecular magnets
Magnetism in DFT calculations, nanostructures, electronic structure methods
Properties of atomic clusters, electronic structure methods
Electronic structure methods, molecular magnetism
Synthesize improved molecular magnet compounds, guided by FLO-SIC calculations of magnet properties. These compounds could be important in applications such as magnetic qubits in quantum computers. The Molecular Magnet research thrust is exploring the interplay of chemical bonding and magnetic properties in molecular magnet compounds. A first objective of this research is to provide experimentally-determined benchmark magnetic exchange coupling data that can be used in the development of the FLOSIC method. One objective is to synthesize new combined 3d, 4d compounds that are expected to have enhanced magnetic anisotropies. Potential applications for these compounds include ultra-high density magnetic storage devices and magnetic qubits for quantum computing.
Bioinorganic chemistry and magnetic applications of multinuclear metal complexes, synthesis and characterization of molecular magnet compounds
Synthesize and characterize MOF-based catalysts, guided by FLOSIC calculations of reaction barriers and pathways. The new MOFs could be used in applications ranging from CO2 capture and converge to the separation of organic molecules. The Transition Metal-based Catalysis research integrates experimental synthesis, and characterization with theory-based computation to study the binding of adsorbates on TM sites in metal-organic-framework (MOF) materials. The first goal of this work is to provide a benchmark set of experimentally-determined adsorption energies to test FLOSIC calculations. Comparisons against these benchmarks will support the development of new implementations of the FLOSIC methodology in the Theory Thrust. The second goal is to develop new and improved MOF-based catalysts for applications such as CO2 capture and conversion and molecular separations.
Clusters and periodic models of transition metal reactions in MOFs, quantum chemistry modeling of catalytic hydrogenation of CO2