Simultaneous Phase Control of Li2 Wave Packets in Two Electronic States

Published

January 1, 2002

Author(s)

H U. Stauffer, J B. Ballard, Z Amitay, S R. Leone

Abstract

State-selective phase control of rotational Li₂ wave packets prepared simultaneously in the E(¹ς_u⁺) and E(¹ς_g⁺) electronic state by resonant impulsive simulated Raman scattering, is demonstrated. Following the initial population of a rovibrational launch state on the A electronic potential energy curve with a cw laser, a single sub-picosecond wave packet preparation pulse centered near 800 nm simultaneously creates a two- state rotational wave packet in the E state (Ņ_E = 18, J_E = 23 and 25) and a three state rotational wave packet in the A state (Ņ_A = 15, J_A = 22, 24, and 26). A temporally delayed 800 nm probe pulse subsequently ionizes both electronic components of the wave packet to allow measurement of the time-dependent coherence in these two electronic states. Via phase manipulation of resonant transition frequencies contained within the preparation pulse, the phases of the E(18,25) and A (15,26) quantum states are either varied concurrently or individually controlled, whereas the phases of the other rovibronic states of the wave packet are in all cases held essentially constant. This phase manipulation is shown to be more complex than a simple additive effect involving the phases applied to the resonant frequencies. These experimental results are compared with the predictions of second order time-dependent perturbation theory. Although systematic discrepancies exist, most likely due to additional phase introduced during the two-photon probe process, once these differences are accounted for, good agreement is found between experiment and perturbation theory.

Citation

Journal of Chemical Physics

Volume

116

Issue

No. 3

Pub Type

Journals

Keywords

coherent control, resonant impulsive stimulated Raman scat

Citation

Stauffer, H. , Ballard, J. , Amitay, Z. and Leone, S. (2002), Simultaneous Phase Control of Li₂ Wave Packets in Two Electronic States, Journal of Chemical Physics (Accessed April 24, 2024)