Density Function Theory Studies of Complex Systems: Structure, Dynamics, and Excited States
EMSL Project ID
35415
Abstract
Our goal is to use DFT approaches to investigate structural and dynamical properties of composite systems by partitioning the underlying elements of such complex systems into the components that are computationally tractable. Projects include solvation studies of actinide ions in polar and non-polar solvents, structure and dynamics of hydrogen storage in nanoparticle frameworks, determination of structure and photoelectron spectrum of molecular systems used in thin-film photovoltaic devices, the role of transition metals in light-harvetsting systems, characterization of hybrid organic-inorganic host systems, and luminescent lanthanide complexes used as optical probes for biomedical imaging applications. These projects overlap critical DoE mission objectives that include increasing the knowledge of the underlying factors that control purification processes for actinides (i.e. nuclear fuels), developing predictability capabilities to assist experiment in the characterization and development of renewable energy resources that includes hydrogen storage and light harvesting systems, characterizing the role of host matrices for alternative lighting systems with an emphasis on organic light emitting diodes, and to develop novel lanthanide-based luminescent materials to provide in vitro and in vivo optical imaging. At least half of these projects are in collaboration with experimental projects where the rest are anticipated to reach out to the experimental community for validation and verification. EMSL computing resources are required as the systems of interest are large with respect to the number of atoms, and with respect to the number of electrons. These projects have been initiated with smaller systems and smaller basis sets. Access to teraflop computing allows for more accurate descriptions as a result of using better basis sets for transition metals and actinides, and using larger systems to study kinetic properties (e.g. diffusion and reaction barriers) in condensed systems where response of the local environment plays a critical role. In addition, recent and ongoing theoretical developments are being incorporated into codes to study systems with difficult electronic structure configurations that are strongly affected by the complex electrochemical environments in which they reside.
Project Details
Project type
Capability Research
Start Date
2009-10-14
End Date
2012-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Ghadar Y, and AE Clark. 2012. "Coupled-cluster, Möller Plesset (MP2), Density Fitted Local MP2, and Density Functional Theory Examination of the Energetic and Structural Features of Hydrophobic Solvation: Water and Pentane ." Journal of Chemical Physics 136(5):054305. doi:10.1063/1.3679933
N.E. Singh-Miller and N. Marzari, 2009. "Surface energies, work functions, and surface relaxations of low index metallic surfaces from first principles", Physical Review B 80(23):235407. DOI:10.1103/PhysRevB.80.235407
N. Peng, Q. Zhang, C.L. Chow, O.K. Tan, and N. Marzari. 2009. “Sensing Mechanisms for Carbon Nanotube Based NH3 Gas Detection”, Nano Letters 9(4):1626-1630. DOI: 10.1021/nl803930w