Methods will be developed to more precisely correlate biomolecule structure in solution to the two fundamental types of observables in an electric birefringence experiment: the amplitude of the signal and the relaxation rates obtainable from the rise and decay of the signal. The numerical methods to be applied, boundary element and finite element calculations, will be used in a unified manner to calculate the observable properties for molecules of arbitrary shape, taking polyelectrolyte effects into account. In polyelectrolytes, the amplitude of the electro-optic signal is dominated by the ion cloud deformation or relaxation. Thus, a crucial aim of this work is to accurately model the ion relaxation effect. The calculations will be tested against Transient Electric Birefringence (TEB) and Optical Kerr Effect (OKE) measurements of short DNA oligomers of known sequence, some of which are cylindrical and others bent, either due to sequence effects or by interaction with small proteins. The saturation birefringence calculations will be supplemented by polarizability calculations in the absence (for OKE) and in the presence (for TEB) of counterions and added salt. Accurate hydrodynamic tensors computed by the boundary element method will yield the relaxation curves of the samples. A critical test of the theories will be the comparison between the relaxation behavior in the two experiments since the signal arises from very different kinds of polarizabilities in the TEB compared to the OKE. Further consistency will be checked by measuring the polarized dynamic light scattering (DLS) correlation function which relaxes with the translational diffusion motion of the macromolecules, and comparison with the predicted relaxation rates. NMR pulsed field gradient methods will also be used for translational diffusion measurements.