Molecular Imaging - Any surprises to be had?
I don't think this is going to put basic quantum chemistry upside down. Because chemistry is complicated, and these tools are "inaccurate". Let me illustrate : it was thanks to spectroscopy of atoms that people discovered the spin of the electron. It then explained a lot of fact that puzzled chemists. A molecule is something awfully complicated, that we can only solve with approximations and powerful computers. So to my mind, molecular observables are unlikely to contradict quantum theories. Now you need the LHC to split particles in order to test the theories. 

This guy will tell you that there are surprises to be had about large molecules, the ones from natural sources (or plain coal) that are a pain in the ass to study by NMR,  or enzymes (like this one, studied with single molecule diffraction).

There will be always surprises. But if we could predict them, would they still be surprises ? (sorry that was too long for a 'comment')