Theory of ultrafast photoinduced electron transfer from a bulk semiconductor to a quantum dot

Andrew M. Rasmussen, S. Ramakrishna, Emily A. Weiss, Tamar Seideman

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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.

Original languageEnglish
Article number144102
JournalJournal of Chemical Physics
Volume140
Issue number14
DOIs
Publication statusPublished - Apr 14 2014

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ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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