We believe that using experimental parameters measured by Raman spectroscopy to guide MD is more powerful and synergistic than using either technique alone. Namely, the bond and dihedral angle parameters measured by Raman spectroscopy provide structural constraints that help guide the construction of starting models and narrow the conformational phase space sampled over the course of the simulation production runs. In addition, the MD simulations provide a powerful method to visualize the three-dimensional structure of amyloid fibrils in a way that cannot be appreciated by only inspecting the bond and dihedral angle distributions measured by Raman spectroscopy. Finally, our work shows that Raman spectroscopy can be used to quantitatively discriminate between different fibril polymorphs.