Learning how to control vibrations in multimode molecules

Summary form only given. We have constructed an automated learning machine to study complex quantum systems. We have used this machine to learn how to selectively excite vibrational modes in a multimode molecule. By using a genetic algorithm to guide a computer controlled optical pulse shaper, we were able to discover what pulse shape would excite a single, selected C-H stretch mode in liquid methanol. The vibrations were excited through stimulated Raman scattering with an intense, shaped, ultrafast laser pulse and they were detected by spectrally analyzing the forward scattered radiation.