MIT Department of Chemistry
Cambridge, MA 02139
mit.edu email: mmavros
Year joined: 2011
|2011||BS in Chemistry and Physics||University of Florida||Advisor: David Micha|
The electrolysis of water is a thermodynamically uphill reaction with a complicated mechanism. While efficient catalysis has extremely important implications for the future of alternative energy, experimental catalytic design is difficult, due to the unclear nature of the mechanism of the oxygen evolution half-reaction. In the past, through QM/MM modeling of transition metal catalysts in water, our group has refined a method for calculating the redox potentials associated with individual mechanistic steps, giving insight into experimentally-observed overpotentials for the oxygen-evolution reaction; unfortunately, this method is extremely computationally demanding.
We are working on a method to be able to computationally predict redox potentials to within about 0.3 V very quickly. Using this procedure, I am studying mechanistically a variety of transition metal oxides within the framework of ligand field theory and make qualitative predictions about their relative catalytic activities. I am also working in collaboration with experimentalists to provide insight into the mechanism of some of the leading experimental water-splitting catalysts.
Ab Initio Dynamics
I am working on a new method to complement existing computational methods for predicting quantum dynamics. Most existing methods (e.g. surface hopping) calculate potential energy surfaces from an exact Hamiltonian and propagate wavepackets "on the fly", leading to approximate dynamics. My project involves taking a different approach: instead of calculating approximate dynamics from an exact Hamiltonian, we can calculate exact dynamics from an approximate Hamiltonian, for which the dynamics are well-defined. My work involves devising a method to map a quantum two-level system interacting with a bath (e.g. electron transfer in solution) on to the Spin-Boson Hamiltonian and propagating dynamics under this Hamiltonian numerically-exactly.