Different possible uses of lasers in crossed beam experiments are examined. The scope is limited to low energy collisions (few tens of meV) between excited atoms and atoms or molecules. The first role of the laser in this kind of experiments is that of a selector, allowing either the preparation of the incoming channel or the analysis of the outcoming one, by selecting one definite atomic level (radiative or metastable), one class of velocities, one magnetic sublevel. In all these applications, the laser does not act on the collision process itself. The situation is quite different at high laser powers and frequencies detuned with respect to atomic frequencies. Some suggestions are made about the feasability of crossed beam studies of these laser-assisted collisions.
We show that multipulse excitation of Rydberg atoms with a sequence of short time-delayed femtosecond pulses results in strong
n selection of the final-state amplitudes. In the experiment, a 150 fs laser pulse, which alone populates
n levels from 22--32 in Li, is chopped into four time-delayed excitation pulses, which results in a strong modification of the
n-level distribution. The mechanism demonstrated in the experiment is derived theoretically: With more pulses, it is shown that the population of a single or a few
n levels can be performed on demand and varied as long as the central laser frequency is given.
We present an approach to laser cooling of internal molecular degrees of freedom for vibrationally hot molecules using a sequence of ultrashort laser pulses. It is assumed that the molecules initially occupy different vibrational states with a substantial portion of the molecules being in excited vibrational states. We show that the ultimate aim of increasing the vibrational ground-state population through a reduction of the system's entropy can be achieved through a multistep process. In the first step, we design an ultrashort laser pulse that selectively transfers most of the population of the excited vibrational states to an excited electronic surface; then the field is switched off and the system allowed to relax until most of the excited electronic state population has decayed due to spontaneous emission. By repeating this procedure a few times, the entropy of the system can be substantially reduced and the population of the vibrational ground state increased considerably, even if the lifetimes of the excited electronic states are much greater than the length of a control pulse, i.e., if dissipative effects are negligiable on the time scales of coherent control.
We consider a gas of two-level atoms of two species (for example, natural Rb vapor consisting of two isotopes) in the field of laser radiation tuned close to resonance with the certain transition of a specific iostope. This radiation may turn to be rather close to a near lying transition of other isotope (within the linewidth of laser radiation), so it is necessary to take into account the possibility of excitation of other isotope in order to evaluate the enrichment degree if it is aimed at the isotope separation by means of selective excitation with subsequent chemcial reaction (in our example the rubidium hydride formation) of the excited isotope which is believed to take place at a rate much higher than that in the ground state of the atom.
We have theoretically investigated the vibrational population transfer in the presence of manifolds of rotational levels in a model 15-level
Li2 molecular system by stimulated Raman adiabatic passage with intense unchirped femtosecond laser pulses. We have considered five rotational levels
Jg=0,2,…,8 associated with the initial vibrational level
vg=0 of the ground electronic state $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$, five rotational levels
Ji=1,3,…,9 associated with the vibrational level
vi=1 of the intermediate excited electronic state $A\text{ }{^{1}\ensuremath{\Sigma}}_{u}^{+}$, and five rotational levels
Jf=0,2,…,8 associated with the final target vibrational levels
vf=1,2 of the $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$ state of the
Li2 alkali dimer. The pump and Stokes laser pulses are taken to have the same temporal (Gaussian) shapes, pulse widths, and linear parallel polarizations. The laser wavelengths are in the (visible) range of 700--740 nm. The (peak) intensities of the pulses are of the order of $1\ifmmode\times\else\texttimes\fi{}{10}^{12}--2.5\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{W}/{\text{cm}}^{2}$ and the pulse widths are of the order of 20--50 fs. We have solved the 15 coupled time-dependent Schr\"odinger equations to study the population transfer to the target-excited vibrational levels. We have observed that, even with ``mushrooming'' of closely spaced rotational levels, efficient and selective population transfer to excited vibrational levels in
Li2 alkali dimer can be achieved for counterintuitive pulse sequence by controlling the pump and Stokes laser parameters. We have endeavored to explain the results within the framework of adiabatic picture.
Efficient excitation of an ensemble of atoms and molecules to a desired state is of fundamental importance not only for spectroscopy but also for quantum control of molecular dynamics in chemical and biological processes. The latter usually occurs on a much shorter time scale (in the femtosecond range) giving rise to steadily advanced problem how to excite one of the nearby levels, even when they are well within the broad fs pulse spectrum. We propose a new effective method for selective excitation of atoms based on the atomic coherence and discuss a sensitive method to verify experimentally the proposed mechanism using the technique of quantum beating in pump-probe experiments.