Dissertation/Thesis Abstract

Theory of the Control of Ultrafast Interfacial Electron Transfer
by Rasmussen, Andrew Musso, Ph.D., Northwestern University, 2015, 137; 3705348
Abstract (Summary)

This dissertation describes the theoretial exploration of electron transfer (ET) processes at the interface between bulk and molecular or nanoscale materials. Analysis of simple model Hamiltonians, those for the two- and three-level electronic systems as well as for a single electronic level coupled to a continuum, inform an understanding of electron transfer in nontrivial systems. A new treatment of the three-level system at an undergraduate level encapsulates the hopping and superexchange mechanisms of electron transfer. The elegance of the behavior of ET from a single-level/continuum system precedes a treatment of the reverse process—quasicontinuum-to-discrete level ET. This reverse process, relevant to ET from a bulk material to a semiconductor quantum dot (QD) offers a handle for the coherent control of ET at an interface: the shape of an electronic wavepacket within the quasicontinuum. An extension of the single-level-to-continuum ET process is the injection of an electron from a QD to a wide-bandgap semiconductor nanoparticle (NP). We construct a minimal model to explain trends in ET rates at the QD/NP interface as a function of QD size. Finally, we propose a scheme to gate ET through a molecular junction via the coherent control of the torsional mode(s) of a linking molecule within the junction.

Indexing (document details)
Advisor: Seideman, Tamar, Weiss, Emily A.
Commitee: Hupp, Joseph T., Schaller, Richard D.
School: Northwestern University
Department: Chemistry
School Location: United States -- Illinois
Source: DAI-B 76/10(E), Dissertation Abstracts International
Subjects: Physical chemistry, Quantum physics
Keywords: Electron transfer, Physical chemistry, Quantum dot, Theoretical chemistry, Torsion, Ultrafast
Publication Number: 3705348
ISBN: 978-1-321-78273-8
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