In recent years interest has significantly quickened in investigation of nonlinear optical and spectroscopic phenomena in such unique objects as Rydberg atoms (the atoms in the energy states near the ionization limit) and van der Waals complexes (dimers). These objects are characterized, in particular, by that their energy states are strongly degenerate due to a large value of angular (rotational) momentum. Here, the problem arises of adequate theoretical description of experimental results, especially when polarization peculiarities of nonlinear radiation processes are considered. The problem is caused by the existence of a huge number of quantum magnetic sublevels of energy states, which are, in the general case, coherently coupled to each other and take part in the radiation processes. Figure 1 gives a vivid presentation of the problem arising even in such a seemingly simple case when one need describe the radiation transitions caused by a strong monochromatic field between two energy levels with large values of the angular momentum J. If the field polarization is arbitrary, the whole set of the magnetic sublevels turn out to be coupled by radiative transitions. Formally, the problem becomes essentially multilevel. In this case not only the hope fades of solving it analytically using the traditional quantum-mechanical approach, but the problems of numerical solution grow abruptly with increasing quantum number J as well. On the other hand, as is often the case, every cloud has a silver lining. With large J we approach the situation when the rotational motion of particles can be described classically. It turns out that the transition from the quantum description of orientation states of the angular momentum to the classical one simplifies the problem radically: it reduces to the problem of radiation processes in the simplest model of nondegenerate states. In this case the rotational motion manifests itself in a dependence of the density matrix elements on orientation angles of the angular momentum as on a parameter.
We have studied polarization effects in the photoassociation of two colliding ultra-cold Na-atoms. In a first step the two colliding atoms absorb a laser photon to associate to a singly excited molecule in a bound state of the 0g− or 1g potential. In a second step the excited molecule absorbs a second photon and is further excited to a bound level in a doubly excited potential (0u− or 1u which are autoionizing). By measuring the produced ions with parallel and perpendicular polarizations of the two laser beams used possible polarization effects can be studied. We find strong polarization effects if a 0g− state is used as the intermediate state and very little or no effects at all if a 1g state is used.
Experimental, polarization-dependent excitation spectra for excited-state-Mg--rare-gas-atom optical collisions are reported. In these first studies of the process, polarized Mg atoms in the 3p
1P1 level are produced by absorption of linearly polarized light tuned to the 3s
1S0\ensuremath{\rightarrow}3p
1P1 resonance transition at 285.2 nm. Detuning-dependent, collision-induced polarization spectra are measured in a \ifmmode\pm\else\textpm\fi{}200-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ range around the Mg 3p
1P1\ensuremath{\rightarrow}5s
1S0 transition at 571.2 nm. The spectra correspond to probing transient Mg-Ne and Mg-Ar molecules on 3p $^{1}\mathrm{\ensuremath{\Pi}}_{1}$\ensuremath{\rightarrow}5s $^{1}\mathrm{\ensuremath{\Sigma}}_{0}^{+}$ and 3p $^{1}\mathrm{\ensuremath{\Sigma}}_{0}^{+}$\ensuremath{\rightarrow}5s $^{1}\mathrm{\ensuremath{\Sigma}}_{0}^{+}$ electronic transitions. Measurements of these excited-state polarization spectra for Mg-Ne optical collisions reveal that for detunings to the red of the atomic Mg 3p
1P1\ensuremath{\rightarrow}5s
1S0 transition, electronic linear polarization greater than 50% survives far into the molecular regime. This represents a direct measure of the polarization important to alignment-dependent inelastic processes in alkaline-earth-metal--rare-gas-atom collisions. The polarization spectra are discussed in terms of existing information on the interatomic potentials and through an axial recoil limit for the polarization degree for parallel and perpendicular molecular transitions. Rate coefficients k for disalignment of Mg 3p
1P1 atoms by collisions with Ar [k=9.4(5)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$
cm3/s] and with Ne [k=6.5(7)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}10}$
cm3/s] are also extracted from the data.
We study laser-intensity effects in two-photon collisional redistribution of radiation. Thereby we concentrate on a special case of recent experimental interest, where the transition from the excited to the final state is saturated by a strong laser field. Both exciting lasers are, however, assumed weak in the sense that the dynamics of a collision between the radiator and a perturber is not significantly influenced by the laser fields. In particular, our treatment explains the intensity independence of the polarization dependence of total fluorescence from the final state which has been measured previously even if the transition from the excited to the final state is saturated.
Experiments were conducted recently (by Weiner and co-workers) on the optical shielding (suppression) of atomic collisions in cold-atom beams, and its variation with the angle between the polarization direction of the shielding light and the direction of approach of the beam. This case is shown here to be a typical example of an optical collision in which quantum interference may persevere between two incident collision partial waves leading to the same output state. This effect depends on the relative collisional phase shift of the two interfering channels, as well as on the angle of approach, and will vanish when averaging over the latter (as with collisions in the bulk). The extent of variation of this interference effect with the relative phase shift is quite broad, and may lead, under favorable conditions, to almost complete shielding at a finite value of the shielding-laser power. The latter observation leaves open the possibility of exerting coherent control over the interference effect in order to optimize the shielding.
The results of double-laser experiments in which
Na2+ and
Na+ are produced in crossed alkali beams under single-collision conditions in the presence of strong optical fields are reported. Structure in the mass-selected product ion intensity as a function laser frequency is observed when the optical field is strongly focused and tuned far off atomic or dimer transitions. These measurements are the first to show that the nuclear motion of the quasimolecular collision intermediate plays an important role in laser-induced collisional ionization.