This award is funded under the American Recovery and Reinvestment Act of 2009 (Public Law 111-5). In this EAGER award, funded by the Experimental Physical Chemistry program, Professors Thomas Skinner and Klaus Woelk and their students will employ optimal control theory as a comprehensive methodology to extend the formidable capabilities of magnetic resonance spectroscopy for research. This research will address current limitations in magnetic resonance spectroscopy: (i) the extreme radio-frequency inhomogeneity seen in toroid cavity probes used in nuclear magnetic resonance (NMR); and (ii) the extreme bandwidths required in electron paramagnetic resonance (EPR). NMR and EPR have a wealth of applications in chemistry, biochemistry, materials science, physics, and medicine that directly benefit society. Achieving objective (i) for the field of toroid cavity NMR will fully enable its unique potential for high pressure and high temperature studies of in-situ chemical reactions and micrometer-scale chemical-shift imaging. Achieving objective (ii) will enable true Fourier transform EPR and its use for structural and conformational studies. In addition, this project will provide postdoctoral training, thesis projects for graduate students, as well as junior and senior projects for physics, chemistry, and engineering majors at Wright State University and Missouri University of Science and Technology. Students and postdoctoral graduates will be educated in state-of-the-art computing and modeling techniques that they may use in potentially unforeseen ways to enhance their viability throughout their prospective careers, positioning them to take advantage of the flexibility in today's job market.