Also,
"Spectrum" is quite vague. What kind of spectra? Atomic emission, absorption, fluorescence, inelastic scattering? There are many things to consider in some of these techniques, such as the probability of several relaxation processes, intermolecular and intramolecular interactions, solvents.
Spectroscopy is a messy thing. If we could simply use DFT and other computational techniques to define everything, then spectroscopists would be out of a job, and monkeys could do the work.
You can get close to predicting what might happen when light interacts with matter, but there is no theory that can define a "spectrum".