Physical Review Letters

Influence of Singlet-Triplet Mixing on the Hyperfine Structure of 5snd Rydberg States in Sr87

R. Beigang, Eckart Matthias, Andre Timmermann

Published Aug 3, 1981• 52 citations

Abstract

A systematic study of the hyperfine structure of $5snd$ $^{1}D_{2}$ and $^{3}D_{2}$ states of $^{87}\mathrm{Sr}$ was carried out by Doppler-free two-photon excitation. In the region of strong singlet-triplet mixing around $n=16$, the hyperfine structure exhibits a marked $n$ dependence which is related to the amount of singlet-triplet mixing.

DOI: 10.1103/physrevlett.47.326

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Physical Review Letters

Influence of Singlet-Triplet Mixing on the Hyperfine Structure of 5snd Rydberg States in Sr87

R. Beigang, Eckart Matthias, Andre Timmermann

Published Aug 3, 1981• 52 citations

Publisher

Abstract

A systematic study of the hyperfine structure of

5snd

^{1}D_{2}

and

^{3}D_{2}

states of

^{87}\mathrm{Sr}

was carried out by Doppler-free two-photon excitation. In the region of strong singlet-triplet mixing around

n=16

, the hyperfine structure exhibits a marked

n

dependence which is related to the amount of singlet-triplet mixing.

DOI: 10.1103/physrevlett.47.326

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A systematic study of the hyperfine structure of

5snd

^{1}D_{2}

and

^{3}D_{2}

states of

^{87}\mathrm{Sr}

was carried out by Doppler-free two-photon excitation. In the region of strong singlet-triplet mixing around

n=16

, the hyperfine structure exhibits a marked

n

dependence which is related to the amount of singlet-triplet mixing.

Doppler-free two-photon spectroscopy was applied to excite hyperfine-induced transitions from the $5{s}^{2}^{1}S_{0}$ ground state to the

F=I

component of the hyperfine multiplet of the

5sns^{3}S_{1}

Rydberg series of

^{87}\mathrm{Sr}

(

n=50,\dots{},85

). The experimental data confirm the interpretation of hyperfine-induced singlet-triplet mixing which is related to the singlet-triplet energy separation.

Singlet-triplet mixing of

4snd ^{1}D_{2}

and

^{3}D_{2}

states of Ca was determined between principal quantum numbers

7<~n<~42

with the use of Doppler-free two-photon spectroscopy. The hyperfine structure of the

4snd ^{1}D_{2}

states was used to probe admixtures of triplet character into the singlet wave functions. It turned out that, in the region of series crossings, an enlarged singlet-triplet mixing was observed.

The hyperfine structure of high Rydberg states of

^{87}\mathrm{Sr}

was studied for principal quantum numbers

80<~n<~150

. The hyperfine interaction causes a strong singlet-triplet mixing between levels with the same total angular momenta

F

but different quantum numbers

n

. Semiempirical calculations show excellent agreement with experiment.

The hyperfine structure of

6snd^{1}D_{2}

Rydberg states of

^{135,137}\mathrm{Ba}

is reported for principal quantum numbers ranging between

n=10

and

n=50

. From our data, singlet-triplet mixing coefficients have been deduced. A three-channel quantum-defect model has been used to analyze the resonance in singlet-triplet mixing of

6snd^{1}D_{2} \mathrm{and} ^{3}D_{2}

Rydberg states in the vicinity of the

5d7d^{1}D_{2}

perturber. For the determination of the scattering matrix, hyperfine-structure data were found to be essential. Good agreement has been achieved between calculated and experimental singlet-triplet mixing coefficients.

The hyperfine structure of the

6snd^{1}D_{2}

(

10<~n<~50

) Rydberg states of barium has been measured and analyzed in terms of singlet-triplet mixing. A dispersionlike resonant behavior of the mixing coefficient $\ensuremath{\Omega}$ was observed for barium and strontium in the vicinity of doubly excited configurations. In barium strong disagreement with multichannel-quantum-defect-theory wave functions was found. The present results are compared with the spin polarization and anisotropy of photoelectrons.