Similar molecules or materials have comparable composition, structure, and other properties thus making them difficult to discriminate for purposes of detection. Although the species may be spectrally similar, they each could have significantly different (quantum) dynamical behavior for detection. Optimal dynamic discrimination (ODD) aims to maximally draw out the differences among similar species by manipulating their molecular dynamics with optimized radiation resources. The highest degrees of discrimination arise upon exploiting control of the quantum dynamics of the species. Theoretical analysis shows that quantum systems differing even infinitesimally in character may be distinguished by means of their dynamics when acted upon by a suitably shaped control field. Simulations have demonstrated the capabilities of optimal discrimination in the presence of laser-pulse noise, signal detection errors, and imperfect signal detection resolution. Recent experiments have demonstrated the feasibility of ODD.