Theory of Conical Intersections and Nonlinear Response:
Our theoretical efforts are very closely tied to the experimental efforts; neither can be successful without the other. The Hamiltonian, being a Hermitian operator, can only support state crossings in N-2 dimensions; therefore, the conical intersection must have a two dimensional branching space. Further, the conical intersection necessarily permits access to multiple product wells. In conjunction with our experimental effort, we intend to map this branching space and observe which nuclear modes are most active in steering the reaction through the branching space. To read this information from the experimental data, we must model the nonlinear response of this system including evolution along the reaction coordinate during the coherence and rephrasing times. To accomplish this task, we will use a combination of high order perturbative models and an auxiliary density matrix non-perturbative approach to model the nonlinear polarization.
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Last Updated:
April 18, 2008
Engel Group
University of Chicago
GCIS E028
929 East 57th Street
Chicago, IL 60637
