A&A 372, 338-345 (2001)
DOI: 10.1051/0004-6361:20010511
F. Rodríguez -
J. A. Aparicio -
A. de Castro -
J. A. del Val -
V. R. González
- S. Mar
Departamento de Optica y Física Aplicada, Facultad de Ciencias, Universidad de Valladolid,47071 Valladolid, Spain
Received 22 January 2001 / Accepted 20 March 2001
Abstract
This work reports a collection of 35 transition probabilities of
lines in the spectral region 450-580 nm, all of them measured
in an emission experiment. Relative intensity measurements have
been made in a pulsed discharge lamp and the absolute Aki values
have been obtained by using reference data taken from the literature.
The electron density has been determined by two-wavelength
interferometry and ranges from 0.1 to
m-3 in the plasma. Temperature (14000-24000 K) has been
simultaneously determined from three different methods, including the
Boltzmann-plot of KrII lines and the KrII/KrI intensities ratios.
The final results have been compared with most of the previous
existing data.
Key words: atomic data - line: profile - plasmas - methods: laboratory
Since 1965, experimental data of transition probabilities of singly-ionized krypton have been obtained. These data should allow researchers to obtain information about atomic structure or the type of coupling to be considered for the theoretical models. However, great discrepancies (Donnelly et al. 1975) exist in the experimental results of the different authors, as well as great uncertainties. In the last ten years there has been a renewed interest in the transition probabilities of KrII. This species has been detected in the spectra of the interstellar medium with help of the Goddard high resolution spectrograph on the Hubble space telescope (Cardelli et al. 1991; Cardelli & Mayer 1997). Krypton represents the material from which the young early type stars are formed (Leckrone et al. 1993). Moreover, krypton is present in many light source and lasers in laboratory studies and in industrial applications (Graves 1983; Mckee et al. 1996).
Although an important number of experimental works (Levchenko 1971; Miller et al. 1972; Podbiralina et al. 1973; Keil 1973; Samoilov et al. 1975; Baessler et al. 1979; Fonseca & Campos 1982; Brandt et al. 1982; Bertuccelli & Di Rocco 1991; Castro et al. 2001) and theoretical works (Koozekanani & Trusty 1969; El Sherbini 1976; Spector & Garpman 1977; Brandt et al. 1982) have been performed to determine Aki-values for KrII, a number of lines in the spectrum exist for which there is no data.
In this work Aki-values have been obtained in an emission
experiment from measurements performed on a linear discharge lamp,
where pure krypton was introduced. The plasma source employed
provides not only all kinds of interferometric and spectroscopic
recordings with great reproducibility in different discharges, but
also makes it possible in a broad range of electron densities
(0.1 to
m-3) and temperatures (14000 to
24000 K). This allows us to acquire reliable spectra for weak
isolated and non-isolated lines, very difficult to obtain
otherwise. Absolute transition probabilities have been obtained
from relative intensity measurements, taking as reference those
from Fuhr & Wiese (1998) and Castro et al.
(2001). In this way, the KrII excitation temperature has
been determined from the Boltzmann-plot. Other techniques to
calculate temperature have also been employed: KrII/KrI intensity
ratios and the algorithm described in Gigosos et al.
(1994). The very good agreement among these three methods
suggests that the plasma is well described by a partial local
thermodynamic equilibrium (pLTE) model (van der Mullen
1990). Other experimental cautions, like the existence of
self-absorption or spectrometer calibration have been carefully
considered. The number of measurements (12) performed for each
line, and its very controlled features, allows us to obtain a very
good set of Aki-values from the mean value and its
uncertainty from the standard deviation, in a spectral interval
where little data exist (450-580 nm), as far as we know. These
values will be compared with those found in literature.
Most of the experimental information relative to the plasma
source, design and management have already been described by
Gigosos et al. (1994), and by del Val et al.
(1998). Here we summarize the specific details concerning
this experiment. An scheme of the experimental set-up is shown in
Fig. 1.
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Figure 1: Experimental arrangement. |
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The source of plasma consists of a cylindrical tube of Pyrex
glass 175 mm in length and 19 mm inner diameter. The lamp has
been designed to avoid sputtering as much as possible. The plasma
was created by discharging a capacitor bank of 20 F charged
up to 7.5 KV. During the whole experiment the lamp was working
with a continuous flow of pure krypton at a rate of 0.82 cm3/min and a pressure of
Pa. In these
conditions the KrII emission lasts approximately 150
s. The
gas was pre-ionized in order to obtain the best discharge
reliability and the necessary equal initial conditions for the
different pulses to be comparable. Spectroscopic and
interferometric end-on measurements were made simultaneously
during the plasma life, and were taken 2 mm off the lamp axis, and
from symmetric positions relative to it (del Val et al.
1998). According to Fig. 1, the lamp is placed in
one of the arms of a Twyman-Green interferometer simultaneously
illuminated with two He-Ne lasers (543.0 nm and 632.8 nm) in
order to determine the electron density evolution curve
from the refractivity changes due to free electrons. The
spectroscopic beam is directed by two pinholes, 2 mm diameter
(D1, D2), separated 1.5 m and focused by a cylindrical lens (L) of
150 mm focal length into the entrance slit of a Jobin-Yvon
spectrometer (1.5 m focal length, 1200 lines/mm holographic
grating), equipped with an optical multichannel analyzer
(O.M.A.). The O.M.A. has a detector array, which is divided into
512 channels (EG&G 1455R-512-HQ).
After a calibration in wavelength, dispersion was measured to be 12.59 pm/channel at 589.0 nm at the first order of diffraction with an uncertainty lower than 1% (Aparicio et al. 1998). A relative intensity calibration of the spectrometer was also very carefully performed. An exhaustive description of the procedures followed can be found in González (1999, 2000). This calibration provides a transmittance function which not only includes the dependence in wavelength of the whole optical system traversed by the spectroscopic beam, but also the different behaviour of the 512 channels of the detector. Its uncertainty has been measured to be lower than 4%.
All measurements were carried out in the first order of
diffraction, the same order for which the calibration in
wavelength and intensity was performed. Time exposure for the
detector was always 5 s. Mirror M3, placed behind the plasma
column, was used to measure the optical depth and to detect
possible self-absorption effects in each line profile. This is
detected in any spectral line if the intensities ratio between
the spectrum taken without mirror M3 and with it is lower at the
peak than at any other part of the profile (González
1999).
As a whole, more than 1000 discharges were performed,
corresponding to 8 different spectral intervals. All KrII lines
were recorded in 12 different instants of the plasma life, with 10
runs for each instant, five with mirror M3, five without. All
measurements were made in the region 450-580 nm. KrII lines were
typically registered in the first 150 s of plasma life, with
the exception of the most intense ones as well as some KrI lines,
which were recorded also up to 240
s after the discharge.
The intensity of the KrI spectral lines increases as the krypton
ions recombine. One example of the spectra recorded can be seen
in Fig. 2. Concerning the interferometric recordings, 15
interferograms for both laser wavelengths were taken at the end
of the experiment, all of them 1 ms long. They have been used to
measure
.
Firstly, for each spectral interval at each instant where
measurements were performed, the average spectra of the five runs
taken with and without mirror M3 were obtained. Averaged spectra
differed from the individual spectra by less than 5%, which gives
a good idea of the reproducibility of the plasma source in
different pulses. By comparing both averaged spectra and using
the algorithms described by González (1999,
2000), it has been possible to detect and reconstruct
spectral profiles when necessary. It is important to note that
self-absorption was detected in less than 10% of the whole
spectral profiles and, in less than 10% of these cases, the
reconstructed profile differed from the measured one without
mirror M3 by more than 20% in the peak intensity. These profiles
have been rejected from further calculations.
![]() |
Figure 2: An example of KrII lines recorded in this experiment. |
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After dividing the averaged spectra by the spectrometer transmittance functions, all of them were fitted to sums of Lorentzian functions plus a luminous background with a linear dependence (Gigosos et al. 1994). This is justified since the Stark effect is the dominant spectral line broadening mechanism at the electron densities achieved in this plasma. Differences between the experimental spectra and the fits were usually lower than 0.5%. The fitting algorithm allows us to determine simultaneously the center, asymmetry, line width and area of each profile. As it can be seen in Fig. 2, even the very overlapped weakest lines have been considered in the fit, not as an objective by themselves, but with the aim of obtaining an accurate measurement of the intensity of their closest isolated spectral profiles. The final uncertainty estimated for the intensity measurement is lower than 15%. This procedures have been apllied to all KrI and KrII lines.
Concerning the 15 measured interferometric recordings, they have
been processed according to the algorithms developed and
described by Aparicio et al. (1998) and de la Rosa et al.
(1990). They allow us to obtain for each wavelength an
average curve of the phase evolution changes along the plasma
life
(i=1, 2) and from them, the
electron density curve
,
according to the expression:
When comparing the
curve measured with the
two-wavelength method (Eq. (1)) with that obtained at a
single wavelength, the differences were always lower than 5%,
which indicate the negligible influence of the bound electrons to
refractivity changes in this plasma. The electron density curve
is shown in Fig. 3, where for each instant, an 10% error
bar has been considered. This is the uncertainty estimated for the
electron density in this work.
![]() |
Figure 3: Electron density evolution curve. An error bar of 10% has been included to the value obtained at each instant of the plasma life. |
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Relative to temperature measurements, it is a common hypothesis to
assume that KrII excitation temperature
,
Saha
temperature and kinetic electron temperature take similar values
in collision-dominated plasmas like those generated in this
experiment (van der Mullen 1990). The KrII excitation
temperature was obtained from the Boltzmann-plot of some KrII
lines, measured in this work, for which the transition
probabilities were known. These Aki-values were taken from
Fuhr & Wiese (1998) and from Castro et al.
(2001). In Table 1, both sets of data are shown and
those employed here are labelled with an asterisk. The criterium
to select the reference data was to use the data from Castro et
al. in all cases except for those lines not measured by them, now
measured, and for which Fuhr and Wiese provide data. It is
important to note that the values from Castro et al.
(2001) were also obtained in an emission experiment by
using as a reference the data from Fuhr & Wiese (1998),
so that the whole set of Aki-values employed in this work
corresponds to the same absolute scale.
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Aki (108 s-1) | Aki (108 s-1) |
(Fuhr & Wiese 1990) | (Castro et al. 2001) | |
457.720 | 0.960 | 0.831* |
458.285 | 0.760 | 0.812* |
461.528 | 0.540 | 0.509* |
461.915 | 0.810 | 0.748* |
481.176 | 0.170* | |
482.518 | 0.190 | 0.208* |
483.207 | 0.730 | 0.787* |
484.660 | 0.762* | |
530.866 | 0.024* | |
533.341 | 0.500* |
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Figure 4: Two examples of a Boltzmann plot performed in different instants of the plasma life. Population of excited states is plotted against the corresponding energy level. |
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Figure 5:
Temperature evolution measured from Boltzmann-plot,
from consecutive krypton intensities ratios and from the
assumption
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Transition | Multiplet | Aki | Ref. | Aki | Ref. |
(nm) | (108 s-1) | (exp) | (108 s-1) | (th) | ||
457.720 | 5s'-5p' | 2D5/2-2F
![]() |
0.741 (12) | This work | 1.415 | Spector & Garpman (1977) |
6.9 | Levchenko (1971) | |||||
1.54 | Miller et al. (1972) | |||||
0.961 | Keil (1973) | |||||
1.05 | Baessler et al. (1979) | |||||
1.23 | Fonseca & Campos (1982) | |||||
0.795 | Brandt et al. (1982) | 1.15 | Brandt et al. (1982) | |||
2.76 | Bertuccelli & Di Rocco (1991) | |||||
0.73 | Samoilov et al. (1975) | |||||
0.831 | Castro et al. (2001) | |||||
0.96 | Fuhr & Wiese (1998) | |||||
458.285 | 5p-6s | 4D
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0.811 (2) | This work | ||
0.812 | Castro et al. (2001) | |||||
0.76 | Fuhr & Wiese (1998) | |||||
459.280 | 5p'-4d'' | 2P
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0.293 (6) | This work | ||
459.849 | 5p-6s | 2P
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0.232 (9) | This work | ||
460.402 | 5p-6s | 4D
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0.420 (11) | This work | ||
461.528 | 5s-5p | 2P3/2-2P
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0.499 (2) | This work | 0.7898 | Koozekanani & Trusty (1969) |
0.87 | Miller et al. (1972) | 0.732 | Spector & Garpman (1977) | |||
0.99 | Podbiralina et al. (1973) | 0.125 | El Sherbini (1976) | |||
0.23 | Samoilov et al. (1975) | |||||
1.55 | Bertuccelli & Di Rocco (1991) | |||||
0.509 | Castro et al. (2001) | |||||
0.54 | Fuhr & Wiese (1998) | |||||
461.915 | 5s-5p | 2P3/2-2D
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0.74 (12) | This work | 0.771 | Koozekanani & Trusty (1969) |
1.47 | Miller et al. (1972) | 0.325 | El Sherbini (1976) | |||
0.808 | Keil (1973) | 1.24 | Spector & Garpman (1977) | |||
0.45 | Samoilov et al. (1975) | |||||
0.817 | Brandt et al. (1982) | 1.24 | Brandt et al. (1982) | |||
1.62 | Bertuccelli & Di Rocco (1991) | |||||
0.748 | Castro et al. (2001) | |||||
0.81 | Fuhr & Wiese (1998) | |||||
479.633 | 5p-6s | 4S
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0.180 (9) | This work | ||
480.297 | 4d-5p' | 4P5/2-2D
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0.006 (12) | This work | ||
481.176 | 5s-5p | 4P1/2-4D
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0.133 (4) | This work | 0.412 | Koozekanani & Trusty (1969) |
0.9 | Levchenko (1971) | 0.166 | Spector & Garpman (1977) | |||
0.46 | Miller et al. (1972) | 0.005 | El Sherbini (1976) | |||
0.32 | Bertuccelli & Di Rocco (1991) | |||||
0.17 | Fuhr & Wiese (1998) | |||||
482.518 | 5s-5p | 2P1/2-4S
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0.246 (5) | This work | 0.073 | Koozekanani & Trusty (1969) |
0.08 | Levchenko (1971) | 0.388 | Spector & Garpman (1977) | |||
0.5 | Miller et al. (1972) | 0.153 | El Sherbini (1976) | |||
0.33 | Podbiralina et al. (1973) | |||||
0.54 | Bertuccelli & Di Rocco (1991) | |||||
0.208 | Castro et al. (2001) | |||||
0.19 | Fuhr & Wiese (1998) |
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Transition | Multiplet | Aki | Ref. | Aki | Ref. |
(nm) | (108 s-1) | (exp) | (108 s-1) | (th) | ||
483.207 | 5s-5p | 4P3/2-4P
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0.896 (12) | This work | 1.061 | Koozekanani & Trusty (1969) |
4.98 | Levchenko (1971) | 1.127 | Spector & Garpman (1977) | |||
1.46 | Miller et al. (1972) | 0.584 | El Sherbini (1976) | |||
1.67 | Bertuccelli & Di Rocco (1991) | |||||
0.787 | Castro et al. (2001) | |||||
0.73 | Fuhr & Wiese (1998) | |||||
483.656 | 5p-5d | 2S
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0.372 (6) | This work | ||
484.660 | 5s-5p | 2P3/2-2P
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0.796 (9) | This work | 1.053 | Spector & Garpman (1977) |
1.75 | Miller et al. (1972) | |||||
2.54 | Podbiralina et al. (1973) | <0.0009 | El Sherbini (1976) | |||
0.898 | Brandt et al. (1982) | 0.36 | Brandt et al. (1982) | |||
2.4 | Bertuccelli & Di Rocco (1991) | |||||
0.762 | Castro et al. (2001) | |||||
530.866 | 5s-5p | 4P3/2-4P
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0.025 (5) | This work | 0.043 | Koozekanani & Trusty (1969) |
0.024 | Fuhr & Wiese (1998) | 0.071 | El Sherbini (1976) | |||
531.741 | 5p-5d | 2D
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0.038 (9) | This work | ||
532.277 | 5p-6s | 2P
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0.042 (5) | This work | ||
533.341 | 4d'-5f | 2D5/2-2F
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0.494 (1) | This work | ||
0.49 | Castro et al. (2001) | |||||
534.676 | 5p-6s | 4D
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0.028 (6) | This work | ||
535.545 | 4d-5f | 2D5/2-4F
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0.018 (9) | This work | ||
541.843 | 4d'-5f | 2D3/2-2D
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0.079 (16) | This work | ||
543.863 | 4d-5p | 4D1/2-4D
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0.058 (29) | This work | ||
544.634 | 4d-5p | 4D1/2-2P
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0.027(9) | This work | ||
546.817 | 4d'-5f | 2D3/2-2F
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0.332(13) | This work | ||
549.954 | 5s-5p | 4P1/2-4P
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0.014 (11) | This work | 0.030 | Koozekanani & Trusty (1969) |
0.021 | El Sherbini (1976) | |||||
553.229 | 4d-5p' | 2F7/2-2F
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0.001 (20) | This work | ||
555.299 | 4d'-5f | 2D3/2-4F
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0.109 (6) | This work | ||
556.865 | 4d-5p | 4D5/2-4D
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0.034 (3) | This work | ||
0.025 | Podbiralina et al. (1973) | |||||
0.025 | Samoilov et al. (1975) | |||||
565.037 | 4d-5p' | 2P3/2-2D
![]() |
0.006 (38) | This work | ||
568.189 | 5s-5p | 2P3/2-4D
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0.100 (8) | This work | 0.314 | Koozekanani & Trusty (1969) |
0.358 | El Sherbini (1976) | |||||
569.035 | 4d-5p' | 2P3/2-2D
![]() |
0.246 (7) | This work | ||
0.082 | Samoilov et al. (1975) | |||||
574.927 | 5p'-5d | 2D
![]() |
0.018 (36) | This work | ||
575.298 | 5s-5p | 2P1/2-4D
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0.014 (8) | This work | 0.037 | Koozekanani & Trusty (1969) |
0.013 | El Sherbini (1976) | |||||
577.141 | 4d-5p | 4D1/2-2P
![]() |
0.086 (8) | This work | ||
577.772 | 4d'-5f | 2F5/2-4F
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0.020 (39) | This work |
Once an Aki-value has been obtained for each line and at
each instant where this line was measured, plots representing all
these values along the plasma life have been made. One of them,
showing the measured transitions probabilities for the KrII
459.28 and 555.299 nm is shown in Fig. 6. As can be seen,
no systematic trends are observed in any of the lines. The random
distribution around the mean value is a typical behaviour in
these measurements. From now on, we will assign the mean value as
the Aki-value and the standard deviation as a quality
indicator of the mean value. In this sense, it is significant
that 28 of the 35 measured KrII lines have uncertainties lower
than 15% and only the 7 weakest lines show greater uncertainties.
This result shows the quality of the measurements performed.
![]() |
Figure 6: Two examples of the evolution of the measured transition probabilities measured in this work along the plasma life. No systematic trends are detected. |
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In Table 2, all measured transitions have been indicated.
They have been ordered by increasing wavelength (first column).
The second and third columns indicate the transition array and
multiplet respectively, in all cases according to the notation
suggested by Striganov & Sventitskii (1968). The fourth
and fifth columns contain all the experimental works considered,
indicating in the case of data coming from this work the
calculated standard deviation (in percentage) in parentheses. It
is important to remark that, in the case of the work from Miller
et al. (1972), this work offers relative transition
probabilities but, since the value for
nm is
coincident with that recommended by Fuhr & Wiese (1998),
both sets of data are comparable between them and of course, with
our data. The sixth and seventh columns contain the
Aki-values obtained from theoretical calculations.
When taking a look at the comparisons among data in Table 2, the first noticeable point is the great scatter in the data. This is a very old problem in KrII transition probabilities, with two different aspects: the absolute scale of the Aki-values compared and the quality of the relative ones. In this work, as explained in Sect. 3.3, the scale selected by us to transform our relative measurements to absolute ones corresponds to that of Castro et al. (2001), which is really the same as that of Fuhr & Wiese (1998). In this last publication, the authors maintain as a reference the same data published by NIST from 1978 (Wiese & Martin 1978, 1980; Fuhr & Wiese 1990, 1996). If we re-examine Fig. 4, we see the nice linear behaviour of the KrII excited states population, a situation always present with our plasma source (e.g. Gigosos et al. 1994; Aparicio et al. 1997; del Val et al. 2000; Mar et al. 2000) and a first result can be guessed. The data from Castro et al. (2001), from Fuhr & Wiese (1998) and therefore, from ourselves, might not be a good absolute scale, but at least does seem to represent a good relative one. Small differences between the data from Castro et al. (2001) and ours, corresponding to measurements performed in the same plasma source, arise from the uncertainty in intensity measurements and statistical deviations of the fits in the Boltzmann plots.
If we compare our data with other experimental ones, we find a
curious agreement with those from Brandt et al. (1982) and
Keil (1973). Both works correspond to measurements
performed in wall-stabilized arcs at atmospheric pressure by
assuming total LTE. Although there are only three data points to
compare with Brandt et al. (1982), the mean ratio between
our data and theirs is 0.91 with only 2% statistical deviation.
The arc at atmospheric pressure is probably one of the plasma
sources closest to LTE and the two-wavelength interferometry
technique employed by them in
diagnostics is one of the
most accurate ones used to determine this parameter. The plasma
generated in our work has been demonstrated to be well described
by a pLTE model and other plasmas generated by this source have
been shown to be very close to LTE (Aparicio et al.
1999). As a conclusion, we can say that the scale from
Brandt et al. (1982) is probably near to the absolute
scale. In relation to data from Miller et al. (1972), very
frequently considered as a good reference in a relative scale, we
do not find good coincidence with our data. In fact, even
assuming that
nm is not a good line to use as the
reference to rescale their work (this is one of the most
prominent lines in KrII visible spectra and is very sensitive to
self-absorption), we find that the ratio between their data and
ours is
%. We can conclude that data from Miller et al. (1972) must be taken with care as a relative scale of
KrII transition probabilities. These comparisons can be shown in
Fig. 7. If we try comparisons with Bertuccelli & Di Rocco
(1991), the mean ratio between their data and ours is
%. Comparisons with other experimental works reveal
greater differences between their relative scales and ours.
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Figure 7: Comparisons between the ratios of data taken from the bibliography (bib) and ours (Tw). Data taken from Table 1 correspond with those labelled with an asterisk there, that is to say, those employed in the Boltzmann plots. For the ratios with these data, 15% error bars have been considered for our results. |
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Relative to theoretical works, comparisons with data from
Koozekanani & Trusty (1969), based on intermediate
coupling calculations with the absolute values obtained from
Hartree-Fock functions, are very poor. Their data are on average
1.87 times greater than ours, with a deviation around 49%.
Discrepancies are even greater when compared to calculations from
El Sherbini (1976). However, we note the very good
coincidence between the conclusions extracted by Brandt et al.
(1982) and ours in relation to calculations performed by
Spector & Garpman (1977), on the basis of intermediate
coupling coefficients with the radial integral obtained from
relativistic self-consistent-field wavefunctions. They found a
mean ratio between their data and those from this theoretical
reference of around
%. Certainly, the present work
contains only three lines measured by Brandt et al.
(1982) as stated before, and four other ones not measured
by them but calculated by Spector & Garpman (1977), but
curiously the mean ratio between this theoretical work and our
data is
%, almost the same as that found by Brandt et al. (1982) with a systematic but reasonable deviation. We
think this result reinforces the idea of a good placing of our
data in a relative scale and is probably not far from an absolute
one.
As a final conclusion, this work offers transition probabilities of a set of 35 KrII lines in the spectral region from 450 to 580 nm. For 20 of them, there are no previous data. We can estimate an error of 15% for more than 80% of them and 40% for the rest, always on a relative scale. Many of them will be useful in refining new calculation models. Furthermore, this work sheds some light what are probably the most significant theoretical and experimental works, those of Spector & Garpman (1977) and Brandt et al. (1982) respectively. However, new and more precise calculations and measurements are still required in order to clarify the uncertainties remaining in KrII transition probabilities.
Acknowledgements
The authors thank S. González for his collaboration in the experimental arrangement, and the Spanish Dirección General de Investigación Científica y Técnica (Ministerio de Educación y Ciencia) and the Consejería de Educación y Cultura de Castilla y León for their financial support under contracts No. PB98-0356 and VA23-99 respectively. Dr. J. A. Aparicio wants to express his personal acknowledgement to the Organización Nacional de Ciegos de España (ONCE) for help.