Geometrical optimization approach to wave packet localization

We derive a variational approach to control the position and dispersion of a vibrational wave packet by optimizing its initial state, proposing different functionals that maximize the probability of finding the wave packet within a predetermined spatial region or minimize deviations of its average position and dispersion with respect to the desired values. Through optical excitation to a photodissociative potential, the method can be used to prepare wave packets at nearly any desired bond length with small dispersion. These wave packets can then be addressed by a second pump pulse to probe otherwise inaccessible molecular configurations and enhance the yield of highly non-Franck-Condon transitions.