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Physical Review A

State changing in collisions of Rb(ns) Rydberg atoms with HF

A. Kalamarides, L. N. Goeller, K. A. Smith, F. B. Dunning, M. Kimura, Neal F. Lane

Published Oct 1, 1987• 22 citations
Publisher

Abstract

Rate constants for state changing in collisions of Rb(ns) Rydberg atoms (40\ensuremath{\le}n\ensuremath{\le}48) with HF molecules have been measured and have been calculated using a semiclassical approach. Agreement between the total rate constants measured experimentally and derived theoretically is very good. The results point to the near-resonant nature of n-changing collisions, but indicate that the rate constants for such reactions are less dependent on energy imbalance than suggested by calculations based on the impulse approximation.

DOI
10.1103/physreva.36.3108

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Inelastic and quasielastic collisions of Rydberg atoms with the heavy rare-gas atoms

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A theory of inelastic n,l-changing and quasielastic l-mixing collisions of Rydberg atoms with the heavy rare-gas atoms is developed. It is based on the semiclassical impact-parameter approach combined with the normalized perturbation theory. Semiclassical formulas for scaled transition probabilities and cross sections as functions of the inelasticity parameter and the collision strength are analyzed. This approach gives a general description of collisional nl\ensuremath{\rightarrow}${\mathit{n}}^{\ensuremath{'}}$ transitions independently of the specific values of the principal quantum number, the relative velocity, and the type of colliding atoms. The energy and angular dependence of the electron-atom scattering amplitude is included in the theory by incorporating the impulse-approximation results in the weak-coupling limit. The Ramsauer-Townsend effect affects significantly the values of the cross sections, especially for the inelastic transitions with large energy transfer. The results obtained are used in calculations of the quenching cross sections for the Rb(nS,nD,nF) atoms in collisions with Ar, Kr, and Xe. Comparison of theory and experiment is made in a wide range of the principal quantum numbers and transition energy defects. \textcopyright{} 1996 The American Physical Society.

Physical Review A•Oct 1, 1996•26 citations
Rate constants for state changing in collisions of Rb(ns) Rydberg atoms (40\ensuremath{\le}n\ensuremath{\le}48) with HF molecules have been measured and have been calculated using a semiclassical approach. Agreement between the total rate constants measured experimentally and derived theoretically is very good. The results point to the near-resonant nature of n-changing collisions, but indicate that the rate constants for such reactions are less dependent on energy imbalance than suggested by calculations based on the impulse approximation.
State-changing in collisions of Rb(nS) - HF are studied using a crossed atomic beam/modulated CW laser technique and selective field ionization for values of principal quantum number n where 40 (LESSTHEQ) n (LESSTHEQ) 49. Collisions between a rotating polar molecule and a Rydberg atom often result in a near-resonant interchange of the rotational energy of the molecule, and a corresponding change in the electronic energy of the atom. A critical parameter is the energy imbalance of the reaction, defined as the difference between the atom's initial and final electronic energy and the molecule's initial and final rotational energy. The molecule used in this experiment, hydrogen fluoride, has a large rotational constant which permits study of n-changing rate constants for transitions from an initially populated s-state to a single n-manifold of high-L states. Because only one final manifold is populated, the reaction involves a single energy imbalance, and thus proves a useful test of theoretical models. n-Changing rate constants for collisions with energy imbalances ranging from 0.057 cm('-1) to 3.447 cm('-1), and ionization and L-mixing rate constants are compared to those predicted by an impulse approximation model and a semiclassical approach.
A theoretical model for the collision of atoms in high Rydberg states (nl) with neutral atoms or molecules is proposed, based on the assumption that the electron-perturber interaction is of very short range compared with the mean radius of the Rydberg atom. A semiclassical method is used to derive a compact expression for the collision probability. The calculations need total cross sections for the scattering of a free and low-energy electron by the perturber. The model is applied to the calculation of a free and low-energy electron by the perturber. The model is applied to the calculation of cross sections for the quenching of n 2 D or n 2 F Rydberg states of Na and Rb by rare-gas atoms of N 2 . On the whole the calculated cross sections are in reasonable agreement with experimental data for n>10 approximately. The model and the results of the calculations are discussed and compared with other theoretical works.
The impact broadening rates of Rb ns Rydberg levels by He, Ar and Xe atoms measured by Weber and Niemax (1982) and by Ne and Kr atoms observed by Thompson et al. (1987) are quantitatively explained over the whole range of the principal quantum number n. As Rb ns Rydberg levels (quantum defect delta =3.13) are very close to the nearly hydrogenic high l levels, inelastic collisions make as important a contribution to the broadening rates as elastic collisions. The authors derive the cross sections for the elastic and inelastic using a combination of Kaulakys' (1984) and Lebedev and Marchenko's (1985) impact theories. Good agreement between the theoretical and experimental broadening rates is achieved over the whole range of n.
Absolute rate constants for ionization of Rb(ns,nd) atoms in collisions with SF6{\mathrm{SF}}_{6}SF6​ have been measured for values of n in the range 38--106. In addition, the kinematics of such reactions have been investigated using Xe(nf) atoms. The data confirm that collisions of Rydberg atoms with targets that attach free low-energy electrons are well described by the ``essentially-free''-electron model. Analysis of the data shows that the cross section \ensuremath{\sigma}(v) for electron attachment to SF6{\mathrm{SF}}_{6}SF6​ at very low electron energies (\ensuremath{\lesssim}10 meV) is inversely proportional to the electron velocity v and, if v is expressed in cm ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$, is given by \ensuremath{\sigma}(v)=(4.2\ifmmode\pm\else\textpm\fi{}1.0)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$/v cm2{\mathrm{cm}}^{2}cm2.
Thermal collisions between Xe(nf) Rydberg atoms and HF molecules have been investigated. The highly excited collision products were detected using selective field ionisation (SFI). Both n-changing and l-changing collisions were identified and the absolute rate constants for these processes, and for collisional ionisation, have been measured for n=26, 27. In addition, the first evidence of molecular rotational excitation through the transfer of energy of electronic excitation from a Rydberg atom is presented.
A theory of inelastic n,l-changing and quasielastic l-mixing collisions of Rydberg atoms with the heavy rare-gas atoms is developed. It is based on the semiclassical impact-parameter approach combined with the normalized perturbation theory. Semiclassical formulas for scaled transition probabilities and cross sections as functions of the inelasticity parameter and the collision strength are analyzed. This approach gives a general description of collisional nl\ensuremath{\rightarrow}${\mathit{n}}^{\ensuremath{'}}$ transitions independently of the specific values of the principal quantum number, the relative velocity, and the type of colliding atoms. The energy and angular dependence of the electron-atom scattering amplitude is included in the theory by incorporating the impulse-approximation results in the weak-coupling limit. The Ramsauer-Townsend effect affects significantly the values of the cross sections, especially for the inelastic transitions with large energy transfer. The results obtained are used in calculations of the quenching cross sections for the Rb(nS,nD,nF) atoms in collisions with Ar, Kr, and Xe. Comparison of theory and experiment is made in a wide range of the principal quantum numbers and transition energy defects. \textcopyright{} 1996 The American Physical Society.