Quantum-State-Sensitive Detection of Alkali Dimers on Helium Nanodroplets by Laser-Induced Coulomb Explosion.

Rubidium dimers residing on the surface of He nanodroplets are doubly ionized by an intense femtosecond laser pulse leading to fragmentation into a pair of Rb^{+} ions. We show that the kinetic energy of the Rb^{+} fragment ions can be used to identify dimers formed in either the X ^{1}Σ_{g}^{+} ground state or in the lowest-lying triplet state, a ^{3}Σ_{u}^{+}. From the experiment, we estimate the abundance ratio of dimers in the a and X states as a function of the mean droplet size and find values between 4∶1 and 5∶1. Our technique applies generally to dimers and trimers of alkali atoms, here also demonstrated for Li_{2}, Na_{2}, and K_{2}, and will enable femtosecond time-resolved measurements of their rotational and vibrational dynamics, possibly with atomic structural resolution.