The International Research Fellowship Program enables U.S. scientists and engineers to conduct three to twenty-four months of research abroad. The program's awards provide opportunities for joint research, and the use of unique or complementary facilities, expertise and experimental conditions abroad.
This award will support a twenty-two-month research fellowship by Dr. Yves A. Mantz to work with Dr. Michele Parrinello at the Eidgenossische Technische Hochschule Zurich (ETH) (Swiss Federal Institute of Technology Zurich) in Switzerland.
The dissociative hydrolysis of dinitrogen pentoxide (N2O5) in both pure water and organic aerosol particles strongly impacts photochemical smog formation by controlling the ozone budget in the troposphere. However, its chemical mechanism is complex, potentially involving the breaking of several bonds, and is not well understood. This important process will be studied by performing atomistic simulation studies of N2O5, water, and malonic acid (HOOCCH2COOH) mixtures, motivated by a very recent experimental study. Several order parameters will be defined in order to distinguish between competing hydrolysis mechanisms, and Car-Parrinello ab initio molecular dynamics (CPAIMD) calculations will be performed in order to sample the configuration space, enabled by state-of-the-art, multidimensional, rare event sampling schemes recently developed by Parrinello and co-workers. The conclusions drawn from the free energy surface will be verified by transition-path sampling calculations and will be useful for subsequent studies of the hydrolysis reaction in interfacial regions.
