_tcm18-11426.gif )
High quality research in physical chemistry, chemical physics and biophysical chemistry.
Subscribers
Non-subscribers
- Purchase article PDF [£27 + taxes]
- Purchase article PDF member offer [£5 + taxes]
Free access
Paper
Phys. Chem. Chem. Phys., 2009, 11, 10293 - 10298, DOI: 10.1039/b912085h
The influence of initial conditions on charge transfer dynamics
Henk Eshuis and Troy van Voorhis
In this work we address the influence of the initial state on electron transfer dynamics by comparing two different ways of setting up the initial state, namely by taking an electron from the HOMO of a DFT ground state, or by using constrained DFT to self-consistently create the initial state. We solve the TDKS equations for the benzyl-pentafluorobenzene cation. The neutral molecule has a localised HOMO, which gives a natural partitioning in donor and acceptor group. We compare the electronic dynamics for varying angle between donor and acceptor and for varying basis set. We show that the methods lead to essentially equivalent results, but that the use of cDFT gives higher currents and a more consistent initial state with respect to variation of basis set and geometry.
RSS feed