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HAL Id: jpa-00221848

https://hal.archives-ouvertes.fr/jpa-00221848

Submitted on 1 Jan 1982

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HIGH RESOLUTION STUDY OF RYDBERG STATES OF BARIUM

E. Eliel, W. Hogervorst

To cite this version:

E. Eliel, W. Hogervorst. HIGH RESOLUTION STUDY OF RYDBERG STATES OF BARIUM.

Journal de Physique Colloques, 1982, 43 (C2), pp.C2-443-C2-446. �10.1051/jphyscol:1982236�. �jpa-

00221848�

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HIGH RESOLUTION STUDY OF RYBBERG STATES OF BARIUM

E.R. Eliel and W. Hogervorst

Natuurkundig Laboratorium, Vrije Univevs-iteit, PB 7161 1081 HV Amsterdam, Holland

Résumé. - Nous avons étudié les séries 6snl, S, P, D et F de 1 atome de baryum avec des lasers à colorant monomodes. La structure de la série F est analysée en tenant compte des interactions électrostatiques, spin-orbite et hyperfine. On montre que l'adjonction d'une interaction effective du type spin-orbite à 2 corps est néces- saire. La structure des niveaux de Rydberg est très sensible à la présence de ni- veaux perturbateurs ce que l'on démontre dans les séries S et F.

Abstract. - We have studied the 6snl S-, P~, D- and F-Rydbergseries of Barium using CW dye lasers. The structure of the F-seri'es is analyzed in terms of the electrostatic repulsion between the two valence electrons, the spin-orbit inter- action and the hyperfine interaction. However, an effective two-body spin-orbit interaction has to be included. The structure of the Rydbergstates is sensitive to the presence of perturbing configurations, as shown in the S- and F-series.

We have performed a high resolution study of the S-, P-, D- and F- Rydberg- series of the alkaline-earth element Barium. The level structure reflects the interaction between the two valence electrons outside closed shells. Configurat- ion interaction with doubly excited states, which influence level positions', Lande-factors and radiative properties ' , affect this structure as was recently shown by Beigang et al.->>° for the D-series of Strontium and by Rinneberg et al.

for the S-series of Barium.

The even-parity Rydbergstates were populated by two-step excitation from the ground state using two stabilized CW dye lasers. In our experimental set-up.which is described elsewhere", the laserbeams perpendicularly intersect a well-colli- mated atomic beam of natural Barium. The first laser is tuned to the 6s2 1S0 •+

6s6p l~?i resonance transition at 553.5 nm and locked to individual hyperfine or isotopic components. The second laser then excites the atoms to the Rydbergstate.

Excitations take place in a field free region and the Rydbergatoms are detected downstream using a field ionization detector. Absorption spectra are obtained by scanning the second laser.

The odd-parity Rydbergseries were directly excited from the metastable 3D j - and

3D2-states at 9034 and 9216 cm with our frequency-doubled CW ring dye laser.9 These states are efficiently populated in a discharge in front of the beam pro- ducing oven.

In this contribution we limit ourselves to a discussion of some results ob- tained for the 1S - and 3F-series.

The structure of the Rydbergstates is expected to be mainly determined by three interactions'^1, the electrostatic^repulsion between the 6s- and nl - electron, the spin-orbit interaction £ i.s of the 1 2 n£-electron and the hyperfine contact interaction a I.s of the 6s-electron (only for the odd isotopes

1 3 5B a and 1 3 7B a with nuclear spin I = 3/2). These interactions are diagram-

matically shown in the upper part of Fig. 1. In a hydrogenic model it is pre- dicted that electrostatic repulsion and spin-orbit interaction scale as n* , where n* is the effective main quantum number. Since the Hyperfine interaction of

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphyscol:1982236

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JOURNAL DE PHYSIQUE

the 6s-electron is constant, at higher 6 5 65

values of n* the three interactions

have to be treated simultaneously.

1 -

- - - - : ; 6 } - - - o - ;

A consequence of the decreasing elec- f

trostatic repulsion and spin-orbit in- el,,t,,,

,,,, ,,,,-,, ,,,

hyportlno

teraction is that the structure of the

odd-isotope Rydbergstates willtonverge 6 5

to the hyperfine structure of the

2 n d

ground-state of the Ba -ion. This is k = n l l

illustrated in Fig. 2. In the up er

part a recording of the transition % l O ~ I . C ~ ~ Y O t w o - b o d y S D I ~ I - ~ r b , t ~ n t o r a c t m n

+ 30f is shown. in the lower Dart of the transitionT3D1 +50f. The -assign

-

merit to the two isotopes 1 3 5 , 1 3 7 ~ ~ FIG. 1 . DIAGRAMMATIC REPRESENTATION OF and the single components of the even THE INTERACTIONS.

isotopes 136'138~a are indicated. The

hyperfine and spin-orbit interaction in the odd isotopes strongly mix the ' ~ 3 , 3~2,3,4-terms resulting in a complicated hyperfine spectrum. With increasing n a clear grouping appears at the high frequency side of the 136'138~a doublet. Each group corresponds to a transition from a specific hyperfine level in 6s5d3Dl. The residual structure within a group reflects the excited state sp$itting,decreasing notably with increasing n and showing the convergence to the Ba - ground state.

In Fig. 2 this grouping does not yet appear at the low-frequency side of the spectrum.

The analysis of the 6sns1s -series is particularly simple due to thg absence of spin-orbit-interactions. In Fig. 3 the

measured position of the odd i s o t ~ ~ e ~ ~ ~ B a with respect to the 138~a-isotope is

plotted, showing an increasing separation as a function of n, whereas the pure iso- tope shift is expected to become constant.

The observed effect is due to the hyper- fine induced mixing of the two levels with total angular momentum F = 312

longing to the

-

and 3 ~ 1 - term bg-

,

expressed by the +nZn -zero matrixelement

- i 1 ~ 0 , F = 3 / 2 1 a I . s 1 3 ~ 1 , F = 3 / 2 > . With increasing n thecsinglet-triplet separat- ion decreases, resulting in a stronger repulsion between the two F= 312- levels.

A calculation along these lines, using known singlet-triplet splittings, results in the smooth curve in Fig. 3. The difference between experimental and cal- culated values in the interval n = 20-30 is constant and equals the isotope shift.

The irregularity at n = 18 is ascribed to the perturber 5d7d1p0, as earlier observed by Rinneberg et al.

.

We observe theonset of a marked irregularity in the interval n = 35

-

40, which is still under study.

The perturber is 5d7d3p1, which interacts strongly with the 3~1-state and thus via the hyperfine interaction, also with the

+v lsO-state.

The analysis of the F-series is more FIG. 2. RECORDINGS OF THE TRANSITION complicated. An attempt to fit the

3 ~ 1 + nf

.

experimental spectra with the three afore

g: LASER GHOST. mentioned interactions with corresponding interaction constants (Slater exchange

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.

good agreement it proved to be necessary to include

n an effective two-body spin-orbit interaction,diagram- matically shown in the lower part of Fig. 1, with interaction constant a. This second order contribut-

30. ion effectively accounts for the configuration inter- action with all neighbouring Rydbergstates of the same series. With the three interaction constants G3,

25 - Snf and a, shown as a function of n* in Fig. 4 in a log-log-plot, the experimental spectra were generally

20. reproduced within 5-10 MHz. As can be seen from this figure, where for convenience the functions n*-3 and n*-4 (n* = n

-

0.17) are also plotted, only for high values of n* the limiting situation of the hydrogenic

Isotope shlft (GHZ C is

Another interesting way of representing the resultsof FIG. 3 . POSITION OF 1 3 7 ~ ~ the F-series is given in Fig. 5. Here part of the WITH RESPECT TO 13sBa IN hyperfine level structure is shown as a function of n.

THE Gsns lSo-SERIES. FULL This figure is constructed in such a way that the F =

CURVE CALCULATED FROM lS0- 112-levels fall on a vertical line. This hyperfine 3~ l - ~ ~ ~ ~ ~ ~quantumnumber occurs only in the 3~p-state, l ~ ~ . thus this hyperfine level is unaffected by hyperfine interactions with 3~3,qand ' ~ 3 . The F = 512, 712 and 912 levels- which start in the lower left section of Fig. 5 cross repeatedly in the region between n = 22 and 35 due to repulsions by nearby F = 512, 712 and 912-1evels.The group of levels F=5/2-1112, which bend off at the right hand side of Fig.5 belong to 3 ~ 4 , the four levels at the top at the right of F = 112 belong to 3 ~ 3 while the remaining levels are 3 ~ 2 . Not shown is the quartet of levels with

IF^-

character. A marked irregularity appears around n = 20, again showing thepresence of a perturber, probably of the type 5d8p3p2.

Acknowledgement. - This work was financially damenteel Onderzoek der Materie.

-+ I n n *

FIG. 4. THE INTERACTION CONSTANTS G ~ ,

Enf

AND a AS A FUNCTION OF n* FOR THE

supported by the Stichting voor Fun-

F-SERIES

.

FIG. 5. THE HYPERFINE STRUCTURE OF

F-STATES AS A FUNCTION OF n.

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JOURNAL DE PHYSIQUE

REFERENCES

See e.g. Aymar M. and Robaux O., J. Phys. B g (1979) 535.

Wynne ~'.J.,/Armstrong J.A. and Esherick P., Phys. Rev. Lett. 39 (1977) 1520.

Aymar M., Champeau R. J., Delsart C. and ~elle; J.C., J. Phys. B z (1981) 4489.

Aymar M., ~rafstrijm P., Levinson C., Lundberg H. and Svanberg S., J. Phys. B s (1982) 877.

Beigang R., Matthias E. and Timmermann A., Phys. Rev. Lett. 47 (1981) 326.

Beigang R., Schmidt D. and Timmermann A., J. Phys. B e (1982)~201.

Rinneberg H., Neukamer J. and Matthias E., Z. Phys. A to be published.

Eliel E.R., Van Leeuwen K.A.H. and Hogervorst W., Phys. Rev.

22

(1980) 1491.

Eliel E.R., Hogervorst W., Van Leeuwen K.A.H. and Post B.H., Opt. Corn.

39 (1981) 41.

Barbier L. and Champeau R.J., J. Physique

2

(1980) 947.

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