Creation control and measurement of large amplitude vibrational wave packets

Summary form only given. We impulsively create vibrational wave packets in CCl/sub 4/, Cl/sub 2/, CO/sub 2/ and SF/sub 6/ using pulses with durations less than the vibrational periods of these molecules inside a hollow core waveguide. The pulses can be shaped using a deformable mirror pulse shaper to selectively excite vibrations. By monitoring the spectrum of a temporally delayed probe pulse, we can observe the dynamics of the wave packets. We observe wave packet dephasing and rephasing as well as rotational dynamics.