Laser-assisted ultrafast photoassociation in HeH2+

•We study numerically photoassociation assisted by femtosecond pulses in HeH2+.•The bond can be formed in a hot collision with the electron initially in H or He+.•We predict Rabi oscillations of the yield as a function of the pulse amplitude.•We predict weak dependence of the yield on the initial nuclear momentum uncertainty.

In this work we report control on the photoassociation of a proton and a Helium cation, or an alpha particle and an Hydrogen atom, to form HeH2+ assisted by strong femtosecond laser pulses. The results follow from the numerical solution of the time-dependent Schrödinger equation using soft-core Coulomb potentials in a (1+1)D model (one dimension for the electronic motion plus one dimension for the nuclear motion) and for a nuclear Hamiltonian describing the dynamics in four electronic states. We study the dependence of the photoassociation yield on the initial nuclear wave function for a hot collision (impact kinetic energy of the order of a eV) and on the laser parameters. We predict high sensitivity on the synchronization of the laser with the collision time and Rabi oscillations for the yield as a function of the pulse amplitude and duration, while the ionization and inelastic scattering can be minimized with pulses of 50 fs or shorter.