The classical trajectory Monte Carlo method has been used to simulate fully stripped ion-circular Rydberg atom collisions. We report that the mechanisms that govern the capture process for ions colliding with aligned Rydberg targets, namely direct and indirect velocity matching, alternate as to which is dominant. Previous experimental and theoretical results for singly charged ion-Rydberg atom collisions demonstrate that direct capture processes dominate at intermediate collision speeds. We have found that for highly charged ion-Rydberg atom collisions electron capture via indirect velocity matching is dominant at intermediate collision speeds and contributes up to 90% of the total capture cross-section.
The classical trajectory Monte Carlo method has been used to simulate fully stripped ion-circular Rydberg atom collisions. We report that the mechanisms that govern the capture process for ions colliding with aligned Rydberg targets, namely direct and indirect velocity matching, alternate as to which is dominant. Previous experimental and theoretical results for singly charged ion-Rydberg atom collisions demonstrate that direct capture processes dominate at intermediate collision speeds. We have found that for highly charged ion-Rydberg atom collisions electron capture via indirect velocity matching is dominant at intermediate collision speeds and contributes up to 90% of the total capture cross-section.
The aim of this work is to investigate the dynamics of collisions between ions and Rydberg atoms by using the Classical Trajectory Monte Carlo (CTMC) method. The study is started by collisions with oriented elliptical Rydberg atom, is then continued to collisions involving hydrogen Rydberg target in an external magnetic field in the l-mixing regime, and later arrives at antihydrogen formation in an external magnetic field where Rydberg positronium is taken as target.\nThe CTMC method has been applied in the study. For different targets, the CTMC method had to be adjusted and reconstructed to properly create the initial target state for the quasi-separable one-body initial system (hydrogen target) and the two-body initial system (positronium target). Charge exchange and ionization cross sections are calculated under special consideration of different initial target states.\nThe velocity matching phenomenon and Thomas capture which appears in the upstream-downstream asymmetry are found in ion-oriented elliptical Rydberg atom collisions, reflecting the important roles of the initial electron spatial and momentum distributions. By increasing the projectile charge, the distortion of the initial states caused by the strong perturbation of approaching projectile induces pronounced changes in the momentum distribution.\nIn the collisions involving hydrogen Rydberg atoms in a magnetic field, a cross section reduction in case of an increasing magnetic field is found for multiply charged projectiles. The structure effect due to the influence of the magnetic field on the initial state distribution results in different capture cross sections for two characterized, kmax and kmin, states. The velocity matching phenomenon as well as the effect of multiply charged projectile ion are observed in the collisions.\nFurthermore, antihydrogen formation in a magnetic field has been studied. Rydberg positroniums are assumed to be the target atoms, colliding with antiprotons. The initial target positronium state is carefully constructed by means of a newly introduced conserved operator, the pseudomomentum K. Similar properties as in the previous hydrogen target atom case were investigated. It is found that the existence of the magnetic field changes the spatial distribution of positronium to irregular motion. By increasing the magnetic field, it induces a decrease of the resulting capture cross sections (i.e. the antihydrogen formation). Thomas capture which happens in the collision plane in the field-free case is foiled. A smaller positronium binding energy and a larger geometrical extension of the target positronium atom yield a larger capture cross section.
Charge-transfer collisions between slow multiply charged ions and highly excited Rydberg atoms have been studied to determine the details of the internal energy transfer accompanying charge exchange. The experiment uses lasers to define uniquely the binding energies of both initial and final states of the collision, thereby eliminating the ambiguity inherent in the selective field ionization method used for previous studies. The results clearly characterize the capture energetics over the range of ion charge q=1−−11 and velocity v=0.031−−0.138a.u. The measurements are in very good agreement with predictions of the classical trajectory Monte Carlo method, but not with predictions of other classical models.
We report a study of charge transfer from laser-aligned Rydberg atoms in collisions with Ar+ ions in the velocity-matching regime. The Rydberg atoms in well-defined magnetic substates were prepared by two-photon laser optical pumping in a weak magnetic field. The results are compared with classical-trajectory Monte Carlo calculations and can also be understood in terms of a simple and ``intuitive'' picture.
Theoretical electron transfer cross sections for 1.3--130 eV/amu singly charged ions colliding with Rydberg atoms (n=28, m=2) in a magnetic field up to 4 T are presented. Both paramagnetic and diamagnetic interactions are taken into account for the initial state and the collision. Cross sections are calculated within the classical trajectory Monte Carlo model. A method to create a classical ensemble of electrons in a nonseparable Hamiltonian allows the initial quantum stationary states to be modeled. The effect of the magnetic field on electron capture is analyzed in terms of the field-induced alteration of the initial state, as well as the direct influence on the collision dynamics.
Thermal collisions between potassium Rydberg atoms with intermediate values of quantum number n and target molecules that capture free low-energy electrons are investigated. The velocity, binding energy, and angular distributions of heavy-Rydberg ion-pair states formed through such collisions are measured. The experimental data are analyzed with the aid of semiclassical Monte Carlo simulations to investigate the dynamics of electron attachment to a variety of target species. Multiple reaction channels involving short- and long-lived intermediates are seen for electron capture by 1,1,1-C2Cl3F3 and CBrCl3 (where dissociation of CBrCl3 intermediates involves production of Br- and Cl- ions). Electron attachment to BrCN produces long-lived BrCN-* intermediates whose dissociation results in the creation of rotationally-hot CN- anions. Electron capture by Fe(CO)5 leads to formation of Fe(CO)5-* intermediates which can fragment producing Fe(CO)4- anions, either directly or after partial redistribution of the excess energy within the intermediate has occurred. Electron transfer in Rydberg atom collisions with C2Cl4 provide no evidence of formation of long-lived C2Cl4 ions, only Cl- ions are seen. Moreover, strong Rydberg atom scattering is observed following collisions of K(12p) Rydberg states with CH3NO2. This finding is consistent with a theory which predicts that collisions between Rydberg atoms with intermediate values of n and polar molecules can lead to strong resonant quenching of Rydberg states, i.e., n and l changing, through formation of short-lived K+...CH3NO2- ion-pair states. Finally, the improvements in sensitivity to electron capture reaction dynamics that might be achieved using different Rydberg species and a crossed molecular beam are examined. Simulations are performed to demonstrate that the use of a hyperthermal helium Rydberg atomic beam and a crossed beam of target molecules such as CCl4, BrCN and CF3I can provide new insights into dissociative electron attachment reactions. The calculations show that not only can much detailed information on translational energy release distributions and intermediate lifetimes be obtained, but also on the electron radial probability density distributions in the Rydberg atoms themselves.
Scattering of K(np) Rydberg atoms by electron-attaching molecules can result in the formation of positive-negative ion pairs through electron transfer reactions. These reactions can involve the dissociation of a transient intermediate negative ion into a smaller negative ion and a neutral fragment, or they can result in the parent molecule forming a metastable negative ion, with the excess energy being distributed among its internal modes. For Rydberg atoms of intermediate n, it is possible for these ion pairs to orbit each other at large separation, weakly bound by their mutual electrostatic attraction, forming what are known as heavy-Rydberg states. Measurements of the binding energy and velocity distributions of the ion pairs are used to probe the dynamics of electron transfer reactions. The data are analyzed using a semiclassical Monte Carlo collision code to explore the lifetime of the intermediate, the nature of its dissociation, the distribution of the excess energy of reaction, and the branching ratio of the various reaction channels. Results obtained using a variety of attaching targets including CF3I, CCl4, SF6, CH2Br2, 1,1,1-C2Cl3F3, CCl3Br, Fe(CO)5, and CH3NO2 have demonstrated both the wide variety of different behaviors that can accompany electron capture as well as the different behaviors of the product ion-pair states themselves. Remarkably, despite previous work showing that it was possible for CH3NO2 to form long-lived valence-bound negative ions through Rydberg electron transfer, the present work showed that such collisions do not result in the formation of long-lived bound ion-pair states. Rather, the data show that collisions lead to very strong Rydberg atom scattering through formation of transient ion-pair states. These results are consistent with theoretical work that predicts significant collisional quenching of Rydberg atoms by highly polar molecules and highlight a new mechanism for Rydberg atom scattering.