Spin is a fundamental property of electrons that helps to define the physics of atoms, molecules, and materials. Although its influence on the ground-state (e.g., magnetism) and optical characteristics of such systems is reasonably well documented, far less is known concerning the extent to which spin influences the chemistry these systems exhibit. Our research program is geared toward the synthesis and characterization of molecular platforms that allow us to probe this question; more specifically, we are interested in the extent to which spin and spin-polarization influences photo-induced energy and electron transfer processes. Our work primarily deals with transition metal-containing compounds and chromophores, and this presentation will highlight our progress in two areas: (1) an examination of spin-selectve energy transfer in synthetically-tailored dinuclear assemblies that provide for a systematic transition from an exchange (i.e., Dexter) to dipolar (Förster) mechanism, and (2) the development of donor-acceptor systems that incorporate Heisenberg spin-coupled metal clusters as a means for modifying the spin angular momentum space accessible for excited-state energy and electron transfer. The synthesis, ground- and excited-state characterization of these systems will be discussed, as well as future directions designed to exploit these phenomena for the creation of molecular wires in which zero-field spin polarization is used to control long-distance electron transfer.

Spin effects on photo-induced electron and energy transfer processes in polynuclear donor-acceptor assemblies

253rd National Meeting (2017)

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