FEMTOCHEMISTRY OF THE LIQUID-PHASE LASER-INDUCED HARPOON REACTION BETWEEN CL-2 AND XE - OBSERVATION OF BOND FORMATION IN REAL-TIME

The liquid phase, two-photon induced intermolecular charge transfer transition, Cl2 + Xe + 2hv --> Xe+Cl2-, in which the photon is resonant with the dissociative Cl2(1PI(u)) intermediate state, is show, to proceed on a time scale shorter than 100 fs. The process is therefore classified as a coherent, cooperative absorption. The subsequent evolution of the harpoon reaction, Xe+Cl2- --> Xe+Cl- + Cl, which in liquid Xe further proceeds to form Xe2+Cl-, is followed in time by stimulating the radiative dissociation of Xe+Cl-. While the formation of Xe+Cl- cannot be temporally resolved, the triatomic bond forms in 330 fs.