Detailed dynamics of direct three-body recombination of singly charged ions.

We consider the main aspects of detailed dynamics of the reactions of direct three-body ion-ion recombination Cs+ + X- + R → CsX + R (X- = F-, I- and R = Ar, Xe) for non-central encounters of the ions. The reactions are simulated by the quasiclassical trajectory method using diabatic semiempirical potential energy surfaces proposed previously. The recombination mechanisms are studied via visualization of randomly selected trajectories for each of the four systems. Comparison of trajectories for different systems with identical sets of initial conditions is carried out. For most of the presented trajectories, the ion encounter energy and the third body energy are equal to 1 eV. The characteristic function of recombination is defined, this function depends on 13 arguments including eight kinematic parameters. It is shown that the transfer of excess energy from the ion pair to the neutral atom can occur, in particular, via an encounter of the R atom with the Cs+ ion, via an encounter of the R atom with the X- ion, or via successive encounters of the R atom with both the ions, as well as via an "insertion" of the R atom between the ions.

Dynamics of third order direct three-body recombination of heavy ions.

The direct three-body recombination reactions Cs+ + X- + R → CsX + R (X = F, I and R = Ar, Xe) are studied within the quasiclassical trajectory method using diabatic semiempirical potential energy surfaces, the encounters of the ions being non-central. The collision energies range between 1 and 10 eV (values typical for low temperature plasma), while the so-called delay parameter, which characterizes the delay in the arrival of the neutral atom R in relation to the time instant when the distance between the ions attains its minimum, is equal to 0 or 20%. The calculation results include the recombination excitation functions, the opacity functions, and the vibrational and rotational energy distributions of the recombination products. All the four reactions considered exhibit similar overall statistical dynamics, but each process has its own features. On the whole, for both the recombining pairs Cs+ + F- and Cs+ + I-, xenon is more effective than argon as an acceptor of excess energy from the ion pair. The rotational energy distributions of the salt molecules CsF and CsI are almost equilibrium, whereas the vibrational energy distributions are strongly non-equilibrium.

Dynamical mechanisms of direct three-body recombination.

Despite the ubiquity of recombination processes in nature and various technologies, presently little is known about the dynamics of these processes. This article reports on a quasi-classical trajectory study of the dynamics of the direct three-body recombination of Cs(+) and Br(-) ions in the presence of a Xe atom at energies of the ion encounter and that of the third body ranging from 0.2 to 10 eV. Several dynamical mechanisms of stabilization of the recombining ion pair have been found. Head-on ion encounters are characterized by two mechanisms of removing the energy from the recombining pair. In the case of nonzero impact parameters of ion encounters, the dynamics leading to the stabilization of the nascent CsBr molecule becomes much more complicated and three new mechanisms appear. They depend mainly on the energy of the ion encounter, on the energy of the collision of the ion pair with the third body, and on the impact parameter of the ion encounter and the impact parameter of the third body. The common feature of all the three mechanisms is the transfer of a fraction of the rotational energy of the recombining pair to the third body. This transfer plays a key role in the stabilization of the molecule. The dynamical peculiarities observed are expected to be common for the recombination of the charged and neutral particles.

XUV laser-plasma source based on solid Ar filament.

We present a laser driven soft x-ray source based on a novel solid argon filament. The continuously flowing micron-sized filament (diameter approximately 56 microm, flow speed approximately 5 mms) was used as a laser target in order to generate a plasma source of high brightness in the "water window" (2.2-4.4 nm) spectral range. The emission properties of the source were characterized in detail with respect to crucial parameters such as positional and energy stability using an extreme ultraviolet (XUV) sensitive pinhole camera and an XUV spectrometer. The results are compared with an argon plasma based on a gas puff target operated under the same experimental conditions showing an increase of the brilliance by a factor of 84. By changing the capillary geometry from a constant diameter to a convergent shape the flow speed of the filament was significantly increased up to 250 mms, facilitating the operation at higher repetition rates.

The complete T-->V,R energy conversion in three-body collisions within the hard sphere model.

It is shown that in hard sphere (impulsive) collisions of atoms with diatomic molecules, complete conversion of the collision energy into the internal energy of the diatomic partner is possible for any number of impacts between the elastic balls representing the particles. The corresponding collision geometries and relations between the masses of the particles are described in detail.

Comparison of experimental time-of-flight spectra of the HF products from the F+H2 reaction with exact quantum mechanical calculations.

High resolution HF product time-of-flight spectra measured for the reactive scattering of F atoms from n-H2(p-H2) molecules at collision energies between 69 and 81 meV are compared with exact coupled-channel quantum mechanical calculations based on the Stark-Werner ab initio ground state potential energy surface. Excellent agreement between the experimental and computed rotational distributions is found for the HF product vibrational states v'=1 and v'=2. For the v'=3 vibrational state the agreement, however, is less satisfactory, especially for the reaction with p-H2. The results for v'=1 and v'=2 confirm that the reaction dynamics for these product states is accurately described by the ground electronic state 1 (2)A' potential energy surface. The deviations for HF(v'=3, j' > or =2) are attributed to an enhancement of the reaction resulting from the 25% fraction of excited ((2)P(12)) fluorine atoms in the reactant beam.

Simulation of the reactive scattering of F+D2 on a model family of potential energy surfaces with various topographies: the correlation approach.

The connection between the salient features of the potential energy surface (PES) and the dynamical characteristics of the elementary collision process is studied using a correlation approach based on quasiclassical trajectory simulations. The method is demonstrated for the reaction F + D2 --> D + DF for which the scattering characteristics were calculated on a model family of PES's based on a London-Eyring-Polanyi-Sato-type five-parameter equation. The correlations between the reactive cross section and the vibrational and rotational quantum numbers and the scattering angle of the DF product, and the various parameters of the collinear and noncollinear PES's, such as the location and height of the minimal barrier and the Sato coefficients, are reported. Although usually correlations between two variables suffice, in some cases coefficients of correlation among three variables are required. The role of nonlinear parameter dependencies in computing the correlation coefficients is also considered. The correlation approach makes it possible to examine a large set of potential surfaces without intermediate human control and obtain quantitative information.

Evidence for a bound HeH2 halo molecule by diffraction from a transmission grating.

The HeH2 van der Waals complex has been identified in a molecular beam produced by a cryogenic (T0=24.7 K) free jet expansion of a 1% H2 mixture in 99% 4He gas. The weakly bound HeH2 complexes in the beam are identified via their first order diffraction angles after passing through a 100 nm period transmission grating. An electron impact mass spectrometer analysis of the diffraction patterns is used to discriminate against ion fragments of the constituent gas clusters.