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Physical Review A

Impact-broadening cross sections of Rydberg levels of alkaline-earth atoms by collision with rare gases at thermal energy

Jun-Qiang Sun, Eckart Matthias, K.-D. Heber, P. J. West, J. Güdde

Published Jun 1, 1991• 10 citations
Publisher

Abstract

Using the wave functions of the multichannel-quantum-defect theory, a semiclassical theory for both elastic and inelastic collisional cross sections of Rydberg atoms, in which there can be more than one valence electron, with ground-state rare-gas atoms is obtained. Especially the noble-gas-induced broadening cross sections of Rydberg series in alkaline-earth atoms can be calculated. An application of theory is shown to explain the irregular broadening rates of Sr 5sns $^{1}$${\mathit{S}}_{0}$ series due to collision with Xe, and a good agreement between theory and experiment is achieved.

DOI
10.1103/physreva.43.5956

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Using the wave functions of the multichannel-quantum-defect theory, a semiclassical theory for both elastic and inelastic collisional cross sections of Rydberg atoms, in which there can be more than one valence electron, with ground-state rare-gas atoms is obtained. Especially the noble-gas-induced broadening cross sections of Rydberg series in alkaline-earth atoms can be calculated. An application of theory is shown to explain the irregular broadening rates of Sr 5sns ^{1}$${\mathit{S}}_{0} series due to collision with Xe, and a good agreement between theory and experiment is achieved.
The author obtains expressions for Rydberg level broadening and shift cross sections and rates suitable for elastic collisions of ground-state rare-gas atoms with Rydberg atoms. The semiclassical impact broadening theory is used. The interaction of a Rydberg atom with a rare-gas atom is approximated by the superposition of polarisation potentials and the Fermi pseudopotential. It is shown that similar expressions for the broadening and shift cross sections due to the perturber-Rydberg-electron interaction can be obtained in the JWKB approximation for the Rydberg-electron wavefunctions and for the square-well model potential. Consequently the shift and width of the Rydberg level are not very sensitive to the shape of the potential but only to its normalisation. Expressions for the shift and width in the square-well potential approximation suitable in the high-density limit of the perturbing atoms are obtained. Limits of the applicability of the expressions for the broadening and shift cross sections are discussed. Calculated broadening and shift rates agree well with experimental results for the broadening and shift of Rydberg levels with small, medium and large principal quantum numbers by all rare gases excepting neon.
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.
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.
Semiclassical calculations of the quasi-elastic l-mixing and inelastic n,l-changing processes in thermal collisions of a Rydberg sodium atom with rare-gas atoms (Ne, Ar, Kr and Xe) as well as and atoms with Ne are presented in a wide range of principal quantum numbers. The main emphasis is put on the study of the effects in the Rydberg-atom - rare-gas-atom collisions associated with both the short- and long-range (polarization) parts of the electron - perturber interaction. It is shown that the polarization interaction between the highly excited electron and the Ne atom provides the major contribution to the cross section of the l-mixing and n, l -changing transitions. We show that the Ramsauer - Townsend effect in slow electron scattering by the heavy rare-gas atoms significantly affects the values of the cross sections, particularly for the inelastic transitions with large energy transfer. A quantitative explanation of these phenomena is given using the recently developed semiclassical normalized perturbation theory for the Rydberg-atom - neutral collisions combined with the modified effective range theory for scattering of slow electrons by the rare-gas atoms.
The impact broadening of Na(nP1/2) (n=6-24), K(nP1/2) (n=8-24) and Rb(nP12/) (n=10-24) levels by noble-gas atoms, N2 molecules and alkali atoms in the ground state has been investigated. Broadening cross sections have been evaluated on the grounds of contributions coming from Rydberg-electron-perturber and ionic core-perturber scattering. Broadening cross sections for Cs(nD3/2)+Cs(6S) collisions for n=11-23 have also been calculated to compare with the experimental ones. Theoretically evaluated broadening cross sections for K(nP12/)+K(4S) and Cs(nD3/2)+Cs(6S) collisions appeared to be in good agreement with existing experimental data.
We have made comprehensive measurements of the noble-gas-induced (He, Ne, Ar, Kr, and Xe) broadening cross sections of the Na $3S\ensuremath{-}nS$ ($3S\ensuremath{-}nD$) transitions, from n=5to38n=5 \mathrm{to} 38n=5to38 (n=4to40n=4 \mathrm{to} 40n=4to40). These measurements were made using the trilevel-echo technique and are an extension and refinement of our earlier work. We find that the cross sections increase as the geometric cross section at low values of nnn, and then, at a value of nnn which depends on the particular noble gas, begin to decrease and eventually reach an asymptotic value at high nnn. The broadening cross sections for the nearly degenerate DDD states are significantly larger than those for the SSS states and clearly show the effect of lll-changing collisions. We also compare our measured SSS-state broadening cross sections with the cross sections calculated using the theory of Omont and find good qualitative agreement.