Development of Novel First Principles Simulations for Reactions at Complex Geochemical Interfaces
EMSL Project ID
51721
Abstract
The proposed development work in this theoretical cross-cutting staff proposal include: (1) Development of new algorithms supporting high-level electron structure calculation of reaction mechanisms involving charge transfer (e.g., electron transfer and proton exchange reactions in partially hydrated mineral surfaces). This software will support the prediction of the mechanisms of electron transfer, the structure of defects in oxides and identify charge transfer mechanisms occurring at the mineral water interface. (2) Development of simulation methods for the interpretation of IR and Raman of the fluid and interface structures. (3) Explore machine learning methods to efficiently sample fluid and interface structure. This software will support proposed EXAFS analysis studies with Rosso and Ilton (EMSL users), as well as other current and future interpretations of vibrational and x-ray spectroscopies in the project. (4) Improving the performance and usability of our codes for geochemistry and environmental researchers, including the continued development of reaction path searching methods. (5) In collaboration with Bagus, develop Software and Modeling strategies to Support Mössbauer Spectroscopy Interpretation (EMSL experimental capability).With its special emphasis on developing new advanced simulation methodology this research addresses DOE OS needs in high-performance computing with a comprehensive focus on unraveling complexity at mineral/fluid interfaces and in disordered materials. Development emphasis is on first principles simulations (forces calculated directly from electronic Schro?dinger equation), providing parameter free predictions applicable to a wide range of temperature, pressure and compositions. The program provides co-workers and the greater geochemical community with innovative massively parallel simulation methods required for geochemical applications.
The ultimate goal is to predict the behaviors of geochemical systems (structure, reactivity and electron transport) reliably in fluid, mineral and low-density phases under arbitrary conditions of temperature and pressure. The theoretical developments of this program will implement advanced computational methods to ensure that EMSL/PNNL remains the leader in computational geochemistry and environmental chemistry. Primary emphasis is on processes at the mineral/fluid interfaces. These interfaces are encountered in many geochemical applications including the formation of ionic species and oxyhydroxide polymers in high and low-density reservoir fluids, acid/base reactions in micro-solvated environments such as the solid liquid interface of transition metal oxide minerals, etc.
Project Details
Start Date
2020-10-12
End Date
2021-09-30
Status
Closed
Released Data Link
Team
Principal Investigator