Picosecond isomerization of a linear triatomic molecule with two intense infrared laser pulses

A two-pulse method of rapid laser induced isomerization of a triatomic molecule is proposed. One laser pulse is resonant with the bending vibration while the second pulse has its frequency close to the stretch mode frequency. Alternatively the second frequency can be set equal to the second harmonic of the first laser. Both lasers are linearly polarized and their polarization vectors are perpendicular. We show from numerical solutions of a two-dimensional, time-dependent Schrِdinger equation, that such perpendicular combination of intense picosecond laser pulses allows the system to follow the reaction path and thus leads to higher isomerization rates.