High vibrational excitation and bond breaking by generalized Raman ladder climbing

By coherent stimulated non-resonant Raman techniques using chirped pulses, it is possible to invert the population between adjacent vibrational levels in a sequence that follows a ladder climbing pattern. Using a realistic model of Na2 we numerically demonstrate the efficiency of the method applied to (1) selective excitation of very highly excited vibrational levels and (2) photodissociation. We explore the different conditions for the optimal performance of the previous goals in the linear chirp regime and we propose and test novel Raman ladder climbing patterns via two or three quantum steps.