Phase Control of Wavepacket Dynamics Using Shaped Femtosecond
R Uberna, Z Amitay, R A. Loomis, S R. Leone
Coherent vibrational and rotational dynamics of the Li2 molecule is controlled by varying the relative phases diameter}n, of the rovibrational wavepacket components, ln>3 -i(ωnt+φn). The coherent superposition is created by excitation of a set of ten rovibronic E1ςg+(nu)E = 12-16 JE = 17, 19) states from an intermediate state, A 1 ςu+(ŅA = 14, JA = 18), using ultrashort optical pulses with well defined spectral amplitudes and phases encoded into the pulse by a liquid crystal spatial light modulator. The wavepacket is probed by time-dependent photoionization and the quantum interference signal is measured as a total ionization yield. The phases of the wavepacket components are optimized to produce partial localization of the wavepacket at a given time t, in specific regions of three-dimensional space defined by the radial and angular coordinates. As a result, the ionization yield, I(t), is maximized or minimized at a time t. The degree of control achieved in the experiment (Imax -Imin = 64( 12%). The experimental data are interpreted in terms of time-dependent radial and angular probability distributions, calculated for different initial conditions that are determined by the phase relationships in the excitation pulse.
femtosecond laser, phase control, wavepacket
, Amitay, Z.
, Loomis, R.
and Leone, S.
Phase Control of Wavepacket Dynamics Using Shaped Femtosecond, Faraday Discussions
(Accessed June 3, 2023)