Authors Accepted Manuscript

Revised Land gJ-factors of some 141Pr II levels

using collinear laser ion beam spectroscopy

S. Werbowy, L. Windholz

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PII: S0022-4073(16)30495-2
DOI: http://dx.doi.org/10.1016/j.jqsrt.2016.10.002
Reference: JQSRT5464
To appear in: Journal of Quantitative Spectroscopy and Radiative Transfer
Received date: 19 August 2016
Revised date: 3 October 2016
Accepted date: 3 October 2016
Cite this article as: S. Werbowy and L. Windholz, Revised Land g J-factors of
some 141Pr II levels using collinear laser ion beam spectroscopy, Journal of
Quantitative Spectroscopy and Radiative Transfer,
http://dx.doi.org/10.1016/j.jqsrt.2016.10.002
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 Revised Lande g J -factors of some 141 Pr II levels using collinear laser ion beam
spectroscopy

S. Werbowya,b,, L. Windholzb
a Institute of Experimental Physics, Faculty of Mathematics, Physics, and Informatics, University of Gdansk, ul. Wita Stwosza 57, PL-80-308 Gdansk, Poland
b Institut f
ur Experimentalphysik, Technische Universitat Graz, Petersgasse 16, 8010 Graz, Austria

Abstract
The Zeeman eect of singly ionized praseodymium spectral lines was studied at small magnetic fields up to 334 G, using
the high-resolution spectroscopic method of collinear laser-ion-beam spectroscopy (CLIBS), where a collimated fast ion beam
is superimposed with a counter propagating laser beam tuned to the desired transition. This nearly Doppler-eect-free technique
enables to observe linewidths as low as 100 MHz and thus to record the Zeeman patterns of the hyperfine structure of the investigated
spectral lines.
From the Zeeman patterns of 21 lines of Pr II lines in the range 570.45 nm to 609.038 nm we have re-determined the Lande
g J -factors of 14 levels of the f 3 d odd and 16 levels of the f 3 p and f 2 d2 even configurations.
The obtained experimental Lande factors are compared with available earlier measurements as well as with theoretical calcula-
tions.
Keywords: Zeeman eect, Lande factors, praseodymium, doppler free laser spectroscopy
PACS: 32.10.Fn, 32.60.+i

1. Introduction Doppler-eect-free laser spectroscopic technique like collinear

In our earlier similar studies on the Zeeman eect of Pr II
lines [1] and Nd II lines [2] we showed for most of the elec-
tronic levels the Lande g J -factors should be treated rather with
cautions. The available experimental data are coming from
classical Doppler-limited spectroscopy and very high magnetic
fields. Most of the available data on the g J factors are from the
early forties of the 20th century [3]. Several decades later Gini-
bre has reinvestigated the Zeeman eect of many Pr II levels
using older available photographic plates [4, 5]. She pointed
out that further studies are needed, due to the complexity of
the Pr spectra. A huge number of lines of neutral as well ionic
Pr are closely spaced or even overlapping, and the accuracy of
the measurements are limited by the only partly known hyper-
fine structure of the combining energy levels. Additionally, the
analysis of the available Zeeman photographic spectrograms,
taken in high magnetic fields (up to 23 000 Gauss) requires that
several transitions had to be considered at one time to interpret
properly the spectra. This has significantly reduced the accu-
racy of the Lande g J factors, most often to 0.05 Lorentz units
[5].
As already mentioned, the extremely rich and dense spec-
trum of Pr and hyperfine structure makes it dicult to inter-
pret properly the observed Zeeman structure and to obtain accu-
rate Lande-g J factors from classical spectroscopy. An adequate
experimental setup to overcome these diculties is a nearly
Corresponding author
Email address: s.werbowy@ug.edu.pl (S. Werbowy)
Preprint submitted to Journal of Quantitative Spectroscopy & Radiative Transfer
laser ion beam spectroscopy (CLIBS). We have already demon-
strated that relatively small magnetic fields (up to few hundreds
Gauss) have minor influence on the ion beam and no observ-
able misalignment between ion beam and laser beam could be
observed. Due to the high spectral resolution, small magnetic
fields are sucient to observe clearly the separation of the Zee-
man components and to determine the Lande factors with good
accuracy. However, like in all high resolution techniques one
has to pay a price for the high resolutions (almost as narrow as
the natural line widths). The price is high complexity of the
experimental setup, the lower signal-to-noise (S/N) ratio and
the limited number of transitions that can be studied. Only
metastable levels of the ground configuration can serve as lower
levels of the excited transitions. Nevertheless, there are alter-
native experimental methods that can complement the CLIBS
investigations and help to determine unknown gj values. Re-
cently we have demonstrated that it is possible to study the Zee-
man eect of rare earth elements in a hollow cathode discharge
lamp using a combination of laser-induced fluorescence (LIF)
and optogalvanic spectroscopy [6, 7]. Although this method is
Doppler-limited with line widths higher than in the CLIBS ex-
periments by at least a factor of 10, it can give access to a larger
number of electronic levels which then can be studied in the
presence of a magnetic field.
Accurate experimental Lande g J -factors are of importance,
because they can help in the theoretical interpretation of the
electronic structure of the element, using i.e. a parametric
multi-configuration approach, which is more accurate than fully
ab initio methods. Blaise et. al. [8] have pointed out that,
October 6, 2016
when performing calculations, even small variations of energy
and Lande factor of the starting level can lead to a bad analy-
sis of the entire complex atomic structure. Pseudo-relativistic
Hartree-Fock (HFR) calculations of g J factors for few even-
parity levels of Pr II have been performed by [9]. Addition-
ally, it was pointed out that in case of Pr II structure the semi-
empirical adjustment of the radial parameters should not be
considered to be taken too seriously due to the scarcity of the
experimental data.
The purpose of this study was to extend the Zeeman eect
studies to a larger amount of Pr II levels. The magnetic field
causes the separation the hyperfine Zeeman components, what
significantly reduces the signal to noise ratio compared to the
field-free recorded hyperfine structure. In order to improve the
S/N ratio in our experiment we needed to increase significantly
the density of the ions in the beam. After some modifications
of our apparatus we have increased the ion beam density by a
factor of 20 or more, what allowed us to study in this work less
intense lines of Pr II.
2. Experiment and computer analysis
The measurements were performed on the CLIBS appara-
tus named MARburg Separator MARS-II, installed originally
at the University of Marburg a.d. Lahn (Germany) and moved
in 2002 to Graz (Austria). For many decades it was used in
studies of the hyperfine interactions and isotope shifts in var-
ious isotopes and elements (including radioactive short lived
isotopes) [10, 11].
Details of the apparatus were described in [1, 12]. However,
in order to increase the density of the ions in the ion beam
we have introduced modifications with respect to the earlier
description. The modifications mainly concerns the part con-
nected with the focusing and guiding of the ion beam. Fig.
1A presents the scheme of the experimental setup with appro-
priate modifications. Nevertheless, the the main components
of the experiment were not changed. Ions were produced in
the evaporation and ionization process in the resistance heated
oven (power consumption <300 W) and then accelerated up to
20 keV. The typical ion current densities could be adjusted by
changing the power of the oven heater reaching the values of
order of 100 nA/mm 2 . This parameter was important in the
experiment, since on one side more heating power of the oven
generated higher ion currents, what resulted in a better S/N ra-
tio, but on the other side overheating burned the cathode tube
where ions are produced. The ion beam formed was guided
into the interaction chamber, where the ions were excited by
the anti-parallel laser beam (a continuous narrow band ring-dye
laser with line width ca. 1 MHz and typical power density 15
mW/mm2 was used). The observed fluorescence was then ob-
served through a Schott glass filter in order to eliminate laser
stray light.
After ionization in the source, ions arrive to the interaction
chamber after 33 s either in the ground or metastable states
belonging to the 4 f 3 6s and 4 f 3 5d odd-parity configurations.
From these levels ions can be excited to higher lying even-parity
2
levels of the e.g. 4 f 2 5d 2 , 4 f 3 6p configurations (for reference
see Fig. 2 from Ref. [1]).
A Doppler tuning technique was used for scanning over
the Zeeman patterns of the investigated transitions. A
praseodymium ions accelerated by a voltage approximately of
UA = 20 kV has a velocity of 165 km/s. By applying a post-
acceleration voltage in the interaction chamber, the kinetic en-
ergy of the ions was increased from the U A level up to (U A +3.5
keV), changeable in steps of as small as 0.35 V, thereby chang-
ing the velocity of the ions in steps of 1.44 m/s. In this way,
a post-acceleration 3.5 keV voltage allows to make a Doppler
scan over the line in a range of appr. 0.77 cm 1 (23 GHz) with
appr. 2.3 MHz resolution.
The magnetic field was produced by two bar-shaped perma-
nent neodymium magnets. We have modified the shapes of the
magnet poles in order to obtain a magnetic field as homogenous
as possible. The permanent magnet bars were connected by the
ferromagnetic bars and placed symmetrically on both sides of
the ion beam, Fig. 1B. This solution was found to be a conve-
nient one since the magnets produced a suciently high mag-
netic field which did not change in time as long as the alignment
of the magnets were not changed.
The absolute value of the magnetic field was measured with a
Hall eect Gauss-meter (Applied Magnetics Laboratory model
GM1A - probe model PB71-10) with an accuracy of 0.25% of
the reading. Additionally, for confirmation we have excited
the Ba II line at 585.368 nm (6p 2 P3/2 5d 2 D3/2 ) transition
(the even isotope 138 (I=0) showing no hyperfine structure was
used). In case of this transition, the g J data are known with
good accuracy: 1.328(8) [13] and 0.7993278(3) [14] for lower
and upper level, respectively.
Fig. 1C presents the distribution of the magnetic field along
the laser-ion interaction region measured by the use of the
Gauss-meter (the width of the probe was 5 mm). As can be
observed from the plot, the magnetic field is not perfectly uni-
form. However, along 2/3 of the excitation path, the magnetic
field does not change by more than 1% of the maximal value in
the center.
From the measurements performed on the Ba II line we have
determined the eective value of the magnetic field. The small
variation of the field along the excitation path resulted only in
a small broadening of the observed Zeeman components. By
changing the alignment of the magnetic bars and their separa-
tion from the interaction region we have established two val-
ues of the magnetic field at which we have recorded the Zee-
man patterns: 235(2) G and 334(3) G. These two values were
selected on the basis of computer simulations of the Zeeman
eect of some Pr II lines. During the preparation phase of the
experiment, we have determined the optimal magnetic field val-
ues - the field should be strong enough to produce a significant
separation of the Zeeman components. Otherwise, the magnetic
field should be not too high in order to avoid a larger deflection
of the ions from the path of the excitation laser and to cause not
a too large separation of the Zeeman components resulting in
an decrease of the signal to noise ratio. From our experience
we can say that convenient values of the magnetic field for 20
keV ion energies are those in the range from 100-400 G.
 The recorded hyperfine-Zeeman patterns were analyzed by
our original software, which has varied the fitted parameters:
the Lande factors, the line shape, background correction and
scaling parameters. The parameters were varied until the cal-
culated structure matched the experimentally observed Zeeman
pattern, minimizing the least squares error sum. This approach
was very eective in studies of various elements, like bismuth
[15, 16, 17], antimony [18, 19] or lead [20].
3. Results
From recordings of 21 lines of 141 Pr II in the region 570.450-
609.038 nm we have re-investigated the Lande g J -factors for
14 odd levels of the ground state configuration f 3 d and 16 even
levels of the configurations f 3 p and f 2 d2 . Because one level
can be involved in several transitions, 8 odd and 6 even levels
were already studied in our preceeding work [1]. Lande factors
for these levels were determined in that work from other lines
and are treated here as control levels. 17 levels presented in this
paper were not studied earlier mainly because of their low S/N
ratio. Fig. 2 presents experimental records of all 21 lines stud-
ied here (M=1, -polarization components) together with
their best fits and the calculated field-free hyperfine structure.
A summary of the obtained Lande-g J factors is presented in
Table 1. The table contains the energy of the level, its classifica-
tion (if the leading component is higher than 60% for the config-
uration and 30% for the term), excitation wavelengths involving
the given level, and experimental values of g J factors obtained
in this work. For comparison, other known values from the liter-
ature are given. It also contains theoretical Hartree-Fock (HFR)
values [9] and semi-empirical least-squares values calculated in
intermediate coupling and provided through the courtesy of an
anonymous Reviewer. The present experimental results are the
mean values from several independent measurements of and
components, recorded in some cases at dierent days and at
dierent transitions. The experimental uncertainties were given
as standard deviation (SD) and standard error (SE) which are
related with each other by formula (SE)=(SD)/ N, where N is
the number of measurements.
4. Conclusions
The presented Zeeman eect analysis of the experimental
spectra of 21 Pr II lines in the weak field regime, having
wavelengths between 570.450 and 609.038 nm (in air), allowed
us to determine accurate Lande-factors of 17 energy levels. To-
gether with the data given in [1] this gives a total of 25 odd
and 31 even levels being re-investigated with the Doppler free
spectroscopy technique of CLIBS.
The present studies are just a tip of an iceberg since for
Pr II ions there are now around 135 odd and 203 even lev-
els known [22]. As was pointed out in [9], theoretical pre-
dictions give rise to 469 possible levels of odd-parity config-
urations (4 f 3 6s, 4 f 3 5d, 4 f 3 6d, 4 f 2 5d 6p, 4 f 2 6s 6p, 4 f 5d 3 ,
4 f 5d 2 6s and 4 f 5d 6s 2 ) with energies up to 30018 cm 1 ,
and 385 even levels belonging to even-parity configurations
3
(4 f 3 6p, 4 f 3 5 f , 4 f 4 , 4 f 2 5d 2 , 4 f 2 6s2 , 4 f 2 6p2 , 4 f 2 5d 6s,
4 f 5d 2 6p and 4 f 5d 6s 6p) with energies up to 35497 cm 1 .
These configurations are expected to be the most significant in
the theoretical interpretation. In this sense we may state that
presently there are only 76 odd (16%) and 198 even (51 %)
levels confirmed experimentally [22].
The experimental data known from literature, presented in
Table 1, are the results of measurements at fields with very high
values, up to 95 000 G [3], moderate fields up to 23 000 G [4]
and quite small fields of few hundreds G fields [1]. In [21] the
opinion is expressed that it is important to work in the weak
magnetic field regime, since then the J value of a level remains
a good quantum number. For very high magnetic fields (in the
direction to the Paschen-Back eect) there could be a distur-
bance of the magnetic components of a level by neighbored en-
ergy levels, having distances comparable to the Zeeman shifts.
Such circumstands must be treated in the analysis of complex
spectra at very high fields.
Comparing the data collected in Table 1, we can conclude,
that most of the Lande factors determined earlier are - within
their relatively high experimental uncertainties - in agreement
with our recent results. However, there are some cases, where
our values dier by more than the experimental uncertainties
from previous values. The discrepancies are also in configura-
tion and term assignments for some even-parity levels. Table 2
collects Pr II even levels investigated in present studies, where
there are two configuration and term assignment present in the
literature, i.e. Ref. [5, 9, 23]. These discrepancies reflect a very
dicult interpretation of the open f -shell configurations in Pr II
structure. Strong correlations and configuration mixing eects
prevent from clear establishing of the level assignment.
In Table 1, deliberately the experimental standard deviation
(SD) of g J is given additionally to SD in order to show that for
all levels our spread of the independent measurement results
(measured by the SD) is smaller than the estimated uncertainty
of 0.05 given in [5]. This concludes that our method to study
the transition with the help of Doppler-free laser spectroscopy
technique at small magnetic fields can provide reliable data of
Lande g J -factors.
Acknowledgments
The present work was supported by Wissenschaftlich-
Technisches Abkommen Osterreich-Polen, projects no.
21/2012 and 12/2014. The interest of Prof. Dr. H.Huhnermann,
University of Marburg/Lahn, is acknowledged. We also would
like to acknowledge the support from an anonymous Reviewer,
who provided us with the semi-empirical intermediate coupling
Lande g J -factor data.
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surements of the 6p 2 P fine-structure levels in Ba138 II using an optical- energy a ration and term, ration and term, ration and term,
induced orientation or alignment of a fast ionic beam. Phys Rev A [cm1 ] from Ref. [5], from Ref. [23], from Ref. [9],
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G. Experimental gJ factor in the metastable 5 D3/2 level of Ba+ . Phys Rev 4 f 3 6p
30018.138 3I 4 f 3 6p 5H 4 f 3 6p 3I
7 7 7
A 1996;54:1199205 29723.998 4 f 3 6p 3K
8 4 f 3 6p ? 4 f 3 6p 3K
8
[15] Werbowy S, Kwela J. The E2 admixtures in mixed multipole lines 459.7 28201.980 4 f 2 5d2 1L
8 4 f 3 6p 5I
8
nm and 461.5 nm in the spectrum of BiI. Eur Phys J-Special Topics 28034.127 4 f 2 5d2 ? ? ?
2007;144:179-84 28009.828 4 f 3 6p 3K
7 4 f 3 6p ?
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of lines of Bi I. J Opt Soc Am B 2014;31:3038-41 26640.915 4 f 2 5d2 ? ? ?
[17] Werbowy S Kwela J. M1-E2 interference in the Zeeman spectra of Bi I. 26445.138 4 f 2 5d2 5K
7 ? ?
Phys Rev A 2008;77:023410 26226.628 ? 5H 4 f 3 6p ? ? ?
4
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man spectra of isotopes 121 Sb and 123 Sb. J Phys B 2010;43:065002 24755.017 4 f 2 5d2 ? 4 f 3 6p ? ? ?
[19] Sobolewski M, Bouazza S, Kwela J. Fine, hyperfine and Zeeman struc-
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4
Figure 1: Experimental setup of MARS-II apparatus with modified magnetic part.

5
Figure 2: Recorded Zeeman-hf structure patterns of the Pr II lines at 235 G. The thin line gray represents the experimental result and the thick black line the
computer best fit. Thin red line presents calculated zero field hyperfine structure of the line. The linewidths are from 50 MHz to 150 MHz. (For interpretation of
the references to color in this figure caption, the reader is referred to the web version of this paper.)

6
 Table 1: Lande-gJ factors of 16 even and 14 odd levels in singly-ionized Praseodymium.
Level Leading Leading Excitation Experimental studies Theoretical studies
energy a onfiguration term wavelength Present studies Ref. [3] Ref. [5] c Ref. [1] HFR Intermediate
[cm1 ] Ref. [5] b Ref. [5] b [nm] gJ (SD)(SE) up to G 23000 G 330 G Ref. [9] coupling e
95000 G

Even levels
30018.138 4 f 3 6p 3I
7 5815.33 1.202 (5) (11) 1.215 1.215 1.211 (16) 1.193 1.182
29723.998 4 f 3 6p 3K
8 5719.09 1.149 (17) (10) 1.145 1.15 1.149 1.154
28816.267 4 f 3 6p 5
K9 5810.58 1.202 (22) (11) 1.217 1.225 1.221
28201.980 4 f 2 5d2 1L
8 5813.55, 6025.72 1.152 (12) (11) 1.154 1.165 1.158 (13) 1.176
28034.127 4 f 2 5d2 ? J=6 5777.291 1.088 (20) (10) 1.13 1.093
28009.828 4 f 3 6p 3K
7 5785.42 1.087 (14) (10) 1.106 1.14
27380.527 4 f 2 5d2 ? J=5 5790.85 1.033 (13) (10) 1.060 1.06
26707.364 ? J=5 6025.82, 6042.87 1.039 (22) (10) 1.07
26640.915 4 f 2 5d2 ? J=5 5791.36 1.054 (15) (10) 1.075 1.03 1.089
26570.206 4 f 2 5d2 ? J=4 5704.5 0.995 (11) (10) 1.05
26445.138 4 f 2 5d2 5K
7 6090.38 1.071 (5) (10) 1.080 1.065 1.096
5
26226.628 ? H4 5818.57 0.874 (43) (16) 0.91 0.887 (10) 0.909 0.902
25467.549 4 f 2 5d2 ? J=4 5756.169, 6087.52 0.886 (36) (9) 0.905 0.90 0.975
24755.017 4 f 2 5d2 ? J=4 5773.165, 5775.90 0.901 (38) (12) 0.911 0.905 0.910 (7) 0.922 0.969
24716.093 4 f 3 6p 5I
5 5786.14, 5788.911 0.898 (15) (8) 0.911 0.915 0.896 (9) 0.920
22675.492 4 f 3 6p 5K
5 5729.42 0.823 (15) (8) 0.821 0.84 0.731 0.776

Odd levels
12826.982 4 f 3 5d 5G
6 5815.33 1.287 (3) (11) 1.285 1.320 (50) 1.269
12243.537 4 f 3 5d 5H
7 5719.09 1.176 (21) (11) 1.18 1.207
11611.054 4 f 3 5d 5I
8 5810.58, 6025.72 1.217 (27) (12) 1.231 1.236 1.225 (11) 1.235
11005.557 4 f 3 5d 5I
7 5813.55 1.156 (8) (10) 1.153 1.15 1.159
10729.778 4 f 3 5d 5H
6 5777.291, 5785.42 1.117 (17) (11) 1.11 1.148
10163.531 4 f 3 5d 3K
6 6042.87 0.924 (14) (9) 0.93 0.920 (8) 0.930
10116.696 4 f 3 5d 5G
4 5790.85, 6025.82 1.050 (22) (10) 1.07 1.031 (10) 1.069
10030.351 3
4 f 5d 3I 6090.38 1.146 (10) (11) 1.14 1.150 (8) 1.149
7
9378.612 4 f 3 5d 5H
5 5791.36 1.029 (16) (9) 1.044 1.05 1.036 (7) 1.050
9045.051 4 f 3 5d 5G
3 5704.5, 5818.57, 6087.52 0.815 (38)(14) 0.83 0.821 (11) 0.834
8099.697 4 f 3 5d 5H
4 5756.169 0.820 (30) (8) 0.83 0.820 (8) 0.848
7446.530 4 f 3 5d 5I
4 5775.9, 5788.911 0.614 (32) (9) 0.622 0.64 0.623
7438.301 4 f 3 5d 3I
5 5773.165, 5786.14 0.852 (22) (9) 0.88 0.865
5226.567 4 f 3 5d 5K
6 5729.42 0.902 (9) (8) 0.915 0.907 0.908
(SD) - Standard deviation, (SE) - Standard error
a
Energy values are taken from [22].
b A configuration name is assigned when its contribution is more than 60%, and an LS term name is assigned when this term totals more than 30%.
c An accuracy of the order of 0.05 Lorentz unit were assumed. [5].
d Observed in ref. [3] g values are in most cases believed to be correct within an average deviation of 0.005 unit.
J
e Semi-empirical intermediate coupling values were provided through the courtesy of an anonymous Collaborator/Reviewer.