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Physical Review A

Combined experimental and theoretical study of the 6p2Pj→8s2S1/2 relative transition matrix elements in atomic Cs

A. Sieradzan, Mark D. Havey, Marianna S. Safronova

Published Feb 6, 2004• 19 citations
Publisher

Abstract

A combined experimental and theoretical study of transition matrix elements of the $6p{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}$ transition in atomic Cs is reported. Measurements of the polarization-dependent two-photon excitation spectrum associated with the transition were made in an $\ensuremath{\approx}200{\mathrm{cm}}^{\ensuremath{-}1}$ range on the low-frequency side of the $6s{}^{2}{S}_{1/2}\ensuremath{\rightarrow}6p{}^{2}{P}_{3/2}$ resonance. The measurements depend parametrically on the relative transition matrix elements, but also are sensitive to far-off-resonance $6s{}^{2}{S}_{1/2}\ensuremath{\rightarrow}\mathrm{np}{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}$ transitions. In addition, as the measured quantities are ratios of polarization-dependent intensities at a single-excitation frequency, they are quite insensitive to a variety of common-mode systematic effects; matrix-element ratios may then be determined to high accuracy. In the past, the matrix-element dependence has yielded a generalized sum rule, the value of which is dependent on sums of relative two-photon transition matrix elements. In the present case, best available determinations from other experiments are combined with theoretical matrix elements to extract the ratio of transition matrix elements for the $6p{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}(j=1/2,3/2)$ transition. The resulting experimental value of 1.423(2) is in excellent agreement with the theoretical value, calculated using a relativistic all-order method, of 1.425(2).

DOI
10.1103/physreva.69.022502

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A combined experimental and theoretical study of transition matrix elements of the 6p2Pj\ensuremath→8s2S1/26p{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}6p2Pj​\ensuremath→8s2S1/2​ transition in atomic Cs is reported. Measurements of the polarization-dependent two-photon excitation spectrum associated with the transition were made in an \ensuremath≈200cm\ensuremath−1\ensuremath{\approx}200{\mathrm{cm}}^{\ensuremath{-}1}\ensuremath≈200cm\ensuremath−1 range on the low-frequency side of the 6s2S1/2\ensuremath→6p2P3/26s{}^{2}{S}_{1/2}\ensuremath{\rightarrow}6p{}^{2}{P}_{3/2}6s2S1/2​\ensuremath→6p2P3/2​ resonance. The measurements depend parametrically on the relative transition matrix elements, but also are sensitive to far-off-resonance 6s2S1/2\ensuremath→np2Pj\ensuremath→8s2S1/26s{}^{2}{S}_{1/2}\ensuremath{\rightarrow}\mathrm{np}{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}6s2S1/2​\ensuremath→np2Pj​\ensuremath→8s2S1/2​ transitions. In addition, as the measured quantities are ratios of polarization-dependent intensities at a single-excitation frequency, they are quite insensitive to a variety of common-mode systematic effects; matrix-element ratios may then be determined to high accuracy. In the past, the matrix-element dependence has yielded a generalized sum rule, the value of which is dependent on sums of relative two-photon transition matrix elements. In the present case, best available determinations from other experiments are combined with theoretical matrix elements to extract the ratio of transition matrix elements for the 6p2Pj\ensuremath→8s2S1/2(j=1/2,3/2)6p{}^{2}{P}_{j}\ensuremath{\rightarrow}8s{}^{2}{S}_{1/2}(j=1/2,3/2)6p2Pj​\ensuremath→8s2S1/2​(j=1/2,3/2) transition. The resulting experimental value of 1.423(2) is in excellent agreement with the theoretical value, calculated using a relativistic all-order method, of 1.425(2).
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We present in this paper results of a nonlinear optical spectroscopy approach to measurement of excited-state transition matrix elements. Recent advances in the quality of excited-state transition matrix elements have permitted renormalization of earlier measurements of transition amplitudes associated with the 5s 2 S 1/2 → 5p 2 P j → 5d 2 D 3/2 two-photon transitions in atomic 87 Rb. Previous measurements were made to high precision, but further improvement of the accuracy was limited by uncertainties in data describing the influence of energetically distant transitions. Availability of more reliable matrix elements, including relativistic all-order calculations of transition matrix elements in alkali atoms, has since significantly improved the situation. In the present paper, we show that theoretical relative transition amplitudes for the excited state 5p 2 P j → 5d 2 D 3/2 doublet (ratio = 1.098(9)) are now in excellent agreement with experiment (ratio = 1.090(6)). This result, combined with our recent work on caesium, shows that it is possible to determine relative line strengths, for transitions connecting atomic excited states, with precision previously found only in state-of-the-art measurements of alkali resonance doublets. Detailed discussion of the experimental technique and supporting data, including polarization measurements on the 5s 2 S 1/2 → 5p 2 P j → 5d 2 D 5/2 transitions, is also presented.
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Results of a theoretical investigation of two-photon, two-color excitation and linear depolarization spectra in atomic cesium are presented. The case of two-beam excitation, where one photon is absorbed through a quadrupole amplitude and the other through a dipole amplitude, is considered. When excitation is through a spin multiplet, the final-state population produced depends sensitively on the relative transition amplitudes through the nondengenerate spin-multiplet terms. In addition, the transition rate contains interference terms depending on the relative directions of the two beams. These terms are manifested strongly when the intermediate states are nonresonant and when the two beams have approximately the same frequency. Application of the results to the 6s2{\mathrm{}}^{2}2S1/2{\mathit{S}}_{1/2}S1/2​\ensuremath{\rightarrow}5d2{\mathrm{}}^{2}2Dj{\mathit{D}}_{\mathit{j}}Dj​\ensuremath{\rightarrow}11p2{\mathrm{}}^{2}2P3/2{\mathit{P}}_{3/2}P3/2​, quadrupole-dipole transition in atomic Cs is made. Polarization-dependent excitation spectra are presented for this case. Effects of hyperfine interactions are also considered.