We describe the preparation of diatomic locations using intense femtosecond laser pulses, and discuss the feasibility of using femtoseond pump-probe techniques to measure the vibrational spectrum of Cl2 3+. Initial attempts to observe the vibrational spectra of Cl2 3+ were unsuccessful. Possible refinements to the experiment are guided by calculations of the electronic states, transition moments, and field-dressed potential curves for Cl2 3+ . Solution of the time-dependent Schrödinger equation using these theoretical data as input allow an accurate simulation of pump-probe experiments and their time-delay signals. Optimization of the experimental parameters via the simulation suggests an improved approach to obtaining the spectra of locations, with special emphasis on the unusual aspects of these systems.

Journal of Physical Chemistry A
Department of Chemistry

Verver, R.J., Matusek, D.R., Wright, J.S, Gibson, G.N., Bhardwaj, R., Aseyev, S., … Ivanov, M.Yu. (2001). Production and study of triply charged diatomic ions with femtosecond pulses: Application to Cl2 3+. Journal of Physical Chemistry A, 105(11), 2435–2443.