Combined Quantum-Classical Theoretical Studies of Processes in the Condensed Phase
Abstract
The proposed work will develop an integrated quantum (QM) and classical theoretical framework that is capable of addressing a number of key problems of importance to the Air Force where reactivity and the surrounding condensed phase media are important. The proposal outlines a few specific example applications including energetic ionic liquids, decomposition and destabilization of solid propellants and heterogeneous catalysis processes related to endothermic fuels. The framework will be completely general, however, and so can be used to examine a range of other problems. The work involves the development of new theoretical tools and the dissemination of these tools in open source software packages available to all users. This includes several advances related to the very accurate renormalized CR-CC(2,3) method, including the derivation and implementation of analytic CR-CC(2,3) gradients and the development of parallel CR-CC(2,3) closed and open shell codes for GAMESS. We will also make several improvements to the effective fragment potential (EFP) method, including the implementation of the term the modeling quadrupole-quadrupole and dipole-octopole interactions and the exchange-repulsion interaction between EFP and QM components. We will also derive and implement the effective fragment molecular orbital (EFMO) charge transfer term. Given an accurate EFMO approach, we will conduct molecular dynamics (MD) simulations with (E)FMO providing the energies and forces. A reactive MC method will also be developed and applied to examine how confinement and condensed phases shift the equilibrium product distribution for reacting systems. These new theoretical advances in quantum and classical simulation methods will be integrated and then applied to several problems of relevance to the Air Force.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- May 30, 2018
- Source ID
- FA95501810321
Entities
People
- Mark S. Gordon
Organizations
- Air Force Office of Scientific Research
- Iowa State University
- United States Air Force