Spectroscopy is a dominant measurement methodology because it resolves molecular level details over a wide concentration range. Its limitations, however, become challenged when applied to complex materials. Coherent multidimensional spectroscopy (CMDS) is the optical analogue of multidimensional NMR and like NMR, its multidimensionality promises to increase the spectral selectivity of vibrational and electronic spectroscopy. This article explores whether this promise can make CMDS a dominant spectroscopic method throughout the sciences. In order for CMDS to become a dominant methodology, it must create multidimensional spectral fingerprints that provide the selectivity required for probing complex samples. Pump-CMDS probe methods separate the pump's measurement of dynamics from a multidimensional and selective probe. Fully coherent CMDS methods are ideal multidimensional probes because they avoid relaxation effects, spectrally isolate the output signals, and provide unique and invariant spectral signatures using any combination of vibrational and electronic quantum states.