Abstract

Ultrafast pump-probe experiments have been applied to the study of vibrational wave-packet dynamics in the excited states of the cesium dimer. Pumping the C(¹П_u)←X(¹Σg⁺) band at several wavelengths between 627 and 650 nm produces a vibrational wave packet with an oscillation period of 600 fs. The wave packet is detected by photoionizing the excited molecule with a time delayed probe pulse. The wave packet oscillations persist for approximately 5 ps, and their decay is attributed to predissociation of the C state. Numerical quantum calculations using the FFT spectral method have been performed on the excited state surface to simulate the time evolution of the wave packet density. Experimental results and simulations for these processes will be presented.

© 1992 Optical Society of America