The resonance Raman spectrum of nitrosyl chloride (CINO) has been measured using excitation wavelengths of 212.5, 219, and 222 nm. These spectra add twelve new vibrational energy levels to the previously-known sixteen levels. A ground state potential energy surface was determined, using a Jacobi coordinate system, resulting in converged energies and wavefunctions for all measured vibrational levels. The resonance Raman spectrum of nitrosyl chloride is interpreted in terms of the dynamics on the electronically-excited potential energy surface. Progress toward a novel scheme for solving the time-dependent Schrodinger equation for the vibrational degrees of freedom of the molecule using a multiwavelet basis set is discussed.