Two-pulse laser control of bond-selective fragmentation

Abstract

We elaborate on a two-pulse (pump-pump) laser control scheme for selective bond-breaking in molecules [Amstrup and Henriksen, J. Chem. Phys. 97, 8285 (1992)]. We show, in particular, that with this scheme one can overcome the obstacle of intramolecular vibrational relaxation. As an example, we consider an ozone molecule with isotopic substitution, that is, 16O16O18O. It is shown that asymmetric bond stretching can be created in simple (intense) laser fields. We predict that an alternating high selectivity between the channels 16O+16O18O and 16O16O+18O can be obtained when such a non-stationary vibrating ozone molecule is photodissociated with short laser pulses (∼10–15 fs) with a time delay corresponding to half a vibrational period (∼17 fs).