title: Theory of ultrafast photoinduced electron transfer from a bulk semiconductor to a quantum dot.
abstract: This paper describes analytical and numerical results from a model Hamiltonian method applied to electron transfer (ET) from a quasicontinuum (QC) of states to a set of discrete states, with and without a mediating bridge. Analysis of the factors that determine ET dynamics yields guidelines for achieving high-yield electron transfer in these systems, desired for instance for applications in heterogeneous catalysis. These include the choice of parameters of the laser pulse that excites the initial state into a continuum electronic wavepacket and the design of the coupling between the bridge molecule and the donor and acceptor. The vibrational mode on a bridging molecule between donor and acceptor has an influence on the yield of electron transfer via Franck-Condon factors, even in cases where excited vibrational states are only transiently populated. Laser-induced coherence of the initial state as well as energetic overlap is crucial in determining the ET yield from a QC to a discrete state, whereas the ET time is influenced by competing factors from the coupling strength and the coherence properties of the electronic wavepacket.
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA.
authors.forename: Andrew M
authors.initials: AM
authors.lastname: Rasmussen
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA.
authors.forename: S
authors.initials: S
authors.lastname: Ramakrishna
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA.
authors.forename: Emily A
authors.initials: EA
authors.lastname: Weiss
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, USA.
authors.forename: Tamar
authors.initials: T
authors.lastname: Seideman