The effect of laser pulse width on Rb2 predissociation is probed. The relative yields of Rb excited state fragments with different pulse widths are compared experimentally. Reproducible dissociation channels are observed.
We present the effects of frequency chirping of laser pulses on (1+1)-photon resonance-enhanced dissociation dynamics of H2. The dissociation occurs via two closely spaced nonadiabatically coupled intermediate levels which are in one-photon resonance or near resonance with the initial level. Predissociating levels embedded into continua are considered. When the first laser field is sufficiently intense and suitably chirped, the dissociation probability is enhanced by adiabatic rapid passage through the avoided crossing arising from the frequency swept radiative interaction. The whole population of the ground level can be effectively transferred to the intermediate levels by this technique facilitating the dissociation process by the second field. We also report the effect of frequency detuning and chirp width on the dissociation probability. Widths of the two peaks of the dissociation line shape increase with an increase in chirp width, resulting in the possibility of control in the dissociation yield. When the first field is a laser pulse of low intensity and constant frequency and the second laser frequency is chirped, predissociating levels take important parts in the dissociation dynamics and we obtain a signature of the nonadiabatic effect of the first step on the second step of photodissociation dynamics. This feature is due to the presence of the predissociating levels and the nonadiabatic mixing of two intermediate levels. All these results can be explained in terms of the adiabatic dressed levels.
We explore the control of the Landau-Zener (LZ) transition in NaI predissociation with low-intensity linearly and quadratically chirped femtosecond far-infrared laser pulses by solving the coupled time-dependent Schrödinger equations. We find that the LZ transition between the excited state and the ground state can be enhanced or be suppressed using a well-delayed control pulse with a proper linear or quadratic chirp. With instantaneously controlling the energy gap, the resonant population inversion induced by Rabi oscillation can facilitate or prohibit the molecular population transfer in the avoided-crossing region. This work provides a deep understanding of coherent control of LZ transition in molecular reaction with chirped femtosecond laser pulses.
Propagation of optical pulses in a resonantly absorbing medium is studied. Propagation time of nanosecond pulses was measured for the Rb D1 transition. At the center of two absorption lines, delay of the pulse peak which is about ten times as large as the pulse width was observed, where zero delay is defined for the propagation with the light velocity in vacuum. On the other hand, at the peak of an absorption line, negative delay was observed for large absorption, where the advance time is as large as 25% of the pulse width. Simulation including the effect of absorption and phase shift reproduced well the experimental results.