Electron spin is a fundamental property of Nature. Although many of the more common physical observables linked to spin are well documented, the degree to which spin and spin polarization permeates the chemistry of molecular systems is not as clear. This presentation will survey our efforts in the design and development of chemical systems that will allow us to determine whether there exists a cause-and-effect relationship between the physical and/or photophysical properties of molecules and their innate spin properties, and if so, to what extent we can exploit this connection in order to manipulate the chemical reactivity of molecular systems. Results from two branches of our research program will be discussed. The first focuses on the use of Heisenberg spin-coupled assemblies as components of donor-acceptor assemblies for probing spin effects in electron and energy transfer processes; in these systems, the thermal accessibility of various spin states created under the influence of spin exchange provides a mechanism for modulating the spin properties of the system absent compositional changes of the donor-acceptor assembly. The second part of the talk will describe the preparation of isotopically labeled Ni<sup>II</sup>-semiquinone complexes and the application of advanced EPR spectroscopies in order to assess the extent to which synthesis can be used to control the spatial distribution of spin density within a molecule.

Spin effects on the physical and photophysical properties of molecular systems

251st National Meeting (2016)

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