When: Tomorrow Friday July 13th from 2 to 3 PM
Where: Cabot Division Room at Mallinckrodt
What: John Parkhill is giving group meeting!
A correlated-polaron electronic propagator: open electronic dynamics
beyond the Born-Oppenheimer approximation
====================================
In this work we develop a theory of correlated many-electron dynamics
dressed by the presence of a finite-temperature harmonic bath. Energy
conversion and transport depend critically on the ratio of
electron-electron coupling to bath-electron coupling, which is a
fitted parameter if a phenomenological basis of many-electron states
is used to develop an electronic equation of motion. Since the present
work doesn’t appeal to any such basis, it avoids this ambiguity. The
new theory produces a level of detail beyond the adiabatic
Born-Oppenheimer states, but with cost scaling like the
Born-Oppenheimer approach. While developing this model we have also
applied the time-convolutionless perturbation theory to correlated
molecular excitations for the first time. Resonant response properties
are given by the formalism without phenomenological parameters.
Example propagations with a developmental code are given demonstrating
the treatment of electron-correlation in absorption spectra, vibronic
structure, and decay in an open system.
--
Ryan Babbush | PhD Student in Chemistry
(949) 331-3943 | babbush(a)fas.harvard.edu
Harvard University | Aspuru-Guzik Research Group
12 Oxford Street, Box 400 | Cambridge, MA 02138
Show replies by date