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Pressure shift and broadening of Rydberg states with high principal quantum numbers (11 ≤ n ≤ 150)

K.-D. Heber, P. J. West, W. Makat, Eckart Matthias

Published Jun 9, 1986• 0 citations
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Abstract

The behavior of alkaline atoms in Rydberg states in the presence of noble gases is a well-known topic.1 Knowledge of pressure shifts and broadening for very high principal quantum numbers is still incomplete, and extension of the data to n values as high as possible seems desirable. We investigated for the first time the shift and broadening of 5 s 21 S 0 → 5 s n d 1 D 2 transitions of 88SrI above n = 100. In those cases, where the Rydberg atoms interact with He, Ar, Kr, or Xe, the observed n dependence of the shift and broadening rates K∆ and Kγ is in agreement with theoretical predictions2 for intermediate n values (20 ≤ n ≤ 50). For high n, however, we cannot verify an asymptotic behavior.

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Physical Review A•Aug 1, 1981•7 citations
The behavior of alkaline atoms in Rydberg states in the presence of noble gases is a well-known topic.1 Knowledge of pressure shifts and broadening for very high principal quantum numbers is still incomplete, and extension of the data to n values as high as possible seems desirable. We investigated for the first time the shift and broadening of 5 s 21 S 0 → 5 s n d 1 D 2 transitions of 88SrI above n = 100. In those cases, where the Rydberg atoms interact with He, Ar, Kr, or Xe, the observed n dependence of the shift and broadening rates K∆ and Kγ is in agreement with theoretical predictions2 for intermediate n values (20 ≤ n ≤ 50). For high n, however, we cannot verify an asymptotic behavior.
Broadening and shift rates for Rb 2S^{2}\mathrm{S}2S and 2D^{2}\mathrm{D}2D Rydberg states with principal quantum number n\ensuremath{\sim}10--50 have been measured for Ne, Kr, and H2{\mathrm{H}}_{2}H2​ perturbers, using the technique of Doppler-free two-photon spectroscopy. From the shift rates at high n, we derived electron scattering lengths of (0.24\ifmmode\pm\else\textpm\fi{}0.01)a0{a}_{0}a0​ for Ne, (-4.0\ifmmode\pm\else\textpm\fi{}0.3)a0{a}_{0}a0​ for Kr, and (1.64\ifmmode\pm\else\textpm\fi{}0.07)a0{a}_{0}a0​ for H2{\mathrm{H}}_{2}H2​. For Ne and Kr, these are in good agreement with other experimental values. Also, the n dependence of broadening and shift rates follows theoretical predictions for Ne and Kr, but not for H2{\mathrm{H}}_{2}H2​.
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.
Collisional broadening and shift data for even parity states of neutral barium are presented. A two-photon absorption technique is used to populate Rydberg states of n d 1 D 2 , 3 D 2 and 1 S 0 series. High-resolution Ba excitation spectra were measured using a diode detector while scanning the frequency of an excimer pumped dye laser. Inert gases Ar, Kr and Xe were used as perturbers at pressures ranging from 10 mb to 400 mb. Shifts and broadenings of spectral lines were measured as a function of pressure and principal quantum number n . Several perturbations and deviations from expected results are discussed in this paper.
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.
Our recent treatment [Phys. Rev. A 18, 1066 (1978)] of the broadening and shift of alkali-metal-atom two-photon $S\ensuremath{-}S$ transitions is applied to the Na $3S\ensuremath{-}\mathrm{nS}$ transitions ($n=6\ensuremath{-}9$) perturbed by Ar, Kr, and Xe rare gases. Comparison with recent experimental data [A. Flusberg et al., Phys. Rev. A 19, 1607 (1979)] on the Na-Ar pair for $n\ensuremath{\le}7$ shows good agreement. However, for transitions to n>8n>8n>8 the calculated pressure effects no longer agree well with experimental data; presumably the pressure effects cannot be adequately described by a simple two-body long-range impact theory.