  Time-resolved Faradary rotation experiments have demonstrated coherent
transfer of electron spin between CdSe colloidal quantum dots coupled by
conjugated molecules. We employ here a Green's function approach, using
semi-empirical tight-binding to treat the nanocrystal Hamiltonian and Extended
Huckel theory to treat the linking molecule Hamiltonian, to obtain the coherent
transfer probabilities from atomistic calculations, without the introduction of
any new parameters. Calculations on 1,4-dithiolbenzene and
1,4-dithiolcyclohexane linked nanocrystals agree qualitatively with experiment
and provide support for a previous transfer Hamiltonian model. We find a
striking dependence on the transfer probabilities as a function of nanocrystal
surface site attachment and linking molecule conformation. Additionally, we
predict quantum interference effects in the coherent transfer probabilities for
2,7-dithiolnaphthalene and 2,6-dithiolnaphthalene linking molecules. We suggest
possible experiments based on these results that would test the coherent,
through-molecule transfer mechanism.
