Direct imaging of direction-controlled molecular rotational wave packets created by a polarization-skewed double-pulse.

High-precision, time-resolved Coulomb explosion imaging of rotational wave packets in nitrogen molecules created with a pair of time-delayed, polarization-skewed femtosecond laser pulses is presented, providing insight into the creation process and dynamics of direction-controlled wave packets. To initiate unidirectional rotation, the interval of the double-pulse was set so that the second, polarization-tilted pulse hit the molecules at the time when molecules were aligned or antialigned along the polarization vector of the first pulse. During the revival period of the rotational wave packet, pulse intervals around both the full and half revival times were used. The observed molecular wave packet movies clearly show the signatures of quantum rotation, such as angular localization (alignment), dispersion, and revival phenomena, during the unidirectional motion. The patterns are quite different depending on the pulse interval even when the angular distribution at the second pulse irradiation is similar. The observed interval-dependence of the dynamics was analyzed on the basis of the real-time images, with the aid of numerical simulations, and the creation process of the packets was discussed. We show that the observed image patterns can be essentially rationalized in terms of rotational period and alignment parameter. Because the double-pulse scheme is the most fundamental in the creation of direction-controlled rotational wave packets, this study will lead to more sophisticated control and characterization of directional molecular motions.

Direct Imaging of Laser-driven Ultrafast Molecular Rotation.

We present a method for visualizing laser-induced, ultrafast molecular rotational wave packet dynamics. We have developed a new 2-dimensional Coulomb explosion imaging setup in which a hitherto-impractical camera angle is realized. In our imaging technique, diatomic molecules are irradiated with a circularly polarized strong laser pulse. The ejected atomic ions are accelerated perpendicularly to the laser propagation. The ions lying in the laser polarization plane are selected through the use of a mechanical slit and imaged with a high-throughput, 2-dimensional detector installed parallel to the polarization plane. Because a circularly polarized (isotropic) Coulomb exploding pulse is used, the observed angular distribution of the ejected ions directly corresponds to the squared rotational wave function at the time of the pulse irradiation. To create a real-time movie of molecular rotation, the present imaging technique is combined with a femtosecond pump-probe optical setup in which the pump pulses create unidirectionally rotating molecular ensembles. Due to the high image throughput of our detection system, the pump-probe experimental condition can be easily optimized by monitoring a real-time snapshot. As a result, the quality of the observed movie is sufficiently high for visualizing the detailed wave nature of motion. We also note that the present technique can be implemented in existing standard ion imaging setups, offering a new camera angle or viewpoint for the molecular systems without the need for extensive modification.