Adiabatic climbing of vibrational ladders using Raman transitions with a chirped pump laser

We present detailed calculations of a new scheme for the adiabatic transfer of population in molecular vibrational ladders and for controlling chemical reactions: Raman chirped adiabatic passage. The scheme makes use of far-off-resonant Raman transitions with one chirped and one monochromatic laser pulse. We show that this method can be used to climb vibrational ladders in molecular systems and, with sufficiently large chirping, can vibrationally dissociate diatomic molecules.