Optical Lines of Ru21+ to Ru24+ Ions

Fan, Junyu; Jiang, Zihuan; Qian, Yuyuan; Liu, Jialin; Xu, Pengcheng; Huang, Liangyu; He, Zhencen; Zou, Yaming; Li, Jiguang; Chen, Chongyang; Yao, Ke

doi:10.3390/atoms10040154

Open AccessArticle

Optical Lines of Ru²¹⁺ to Ru²⁴⁺ Ions

by

Junyu Fan

^1,2,

Zihuan Jiang

¹,

Yuyuan Qian

¹,

Jialin Liu

¹,

Pengcheng Xu

¹,

Liangyu Huang

¹,

Zhencen He

¹

,

Yaming Zou

¹,

Jiguang Li

³

,

Chongyang Chen

¹ and

Ke Yao

^1,*

¹

Shanghai EBIT Laboratory, and Key Laboratory of Nuclear Physics and Ion-Beam Application (MOE), Institute of Modern Physics, Fudan University, Shanghai 200433, China

²

Department of Applied Sciences, Delft University of Technology, 2628 CJ Delft, The Netherlands

³

Institute of Applied Physics and Computational Mathematics, Beijing 100088, China

^*

Author to whom correspondence should be addressed.

Atoms 2022, 10(4), 154; https://doi.org/10.3390/atoms10040154

Submission received: 31 October 2022 / Revised: 6 December 2022 / Accepted: 14 December 2022 / Published: 15 December 2022

(This article belongs to the Special Issue 20th International Conference on the Physics of Highly Charged Ions)

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Abstract

:

In this work, we report a spectroscopy measurement of Ru

^{21 +}

to Ru

^{24 +}

ions in the optical region using a low energy electron beam ion trap. Twelve lines were observed. The multiconfiguration Dirac–Hartree–Fock and relativistic configuration interaction methods were used to calculate the atomic level energies and the transition rates. With the assistance of the theoretical results, eleven magnetic dipole lines were identified. The experimental results provide new reference data for further theoretical investigations of the complex ions.

Keywords:

Ru ions; magnetic dipole lines; EBIT; MCDHF

1. Introduction

The development of high-resolution spectrograph techniques in the optical region allows us to unambiguously identify the spectral lines emitted from complex highly charged ions and perform high precision measurement. It is valuable in various applications, for instance, diagnostics of properties of terrestrial and astrophysical plasma [1,2,3,4], tests of quantum electrodynamics (QED) effects in many electron systems [5,6], and analyses of the atomic level splitting for further developing highly charged ion-based atomic clocks [7,8,9,10], etc.

Due to the complex structure of an open 3d subshell, strong electron correlation effects exist in the 3d

^{n}

configurations, in which n is the number of electrons in the 3d subshell. Accurate calculations of the atomic energy levels are still challenging, attracting much attention in these systems experimentally and theoretically [11,12,13,14,15,16,17,18,19,20,21,22,23,24,25]. Great success has been achieved. For instance, a large-scale multiconfiguration Dirac–Hartree–Fock method was used in studying the energy levels of the 3d

^{n}

(n = 1–9) configurations of tungsten ions [25], and core correlation effects were found to be important. Zhang et al. [19] calculated the

n = 3

transition energies of W

^{47 +}

–W

^{55 +}

within 0.1% accuracy compared with the experimental value [12] and predicted strong magnetic dipole transition lines in the tungsten ions. However, in the low-Z side, discrepancies between the experimental and calculated results exist [21,23], especially in the 3d

^{n}

ground configurations. Some significantly large discrepancies were also found along the calcium isoelectronic sequence [21], which hints at the necessity of a reanalysis of the experimental results. In medium heavy ions, very few experiments are available. Experimental reference data are needed for comparisons.

In the case of Ru

^{21 +}

–Ru

^{24 +}

ions, the ground configurations are 3

d^{5}

, 3

d^{4}

, 3

d^{3}

, and 3

d^{2}

, respectively. A number of forbidden transitions connect the energy levels within the ground configurations, part of which correspond to the wavelengths that fall into the optical region. To the best of our knowledge, there are no experimental results available for these ions. In the present work, we reported on the measurement of the magnetic dipole lines from Ru

^{21 +}

–Ru

^{24 +}

ions in a low-energy electron beam ion trap. The corresponding atomic-structure calculations were carried out with the multiconfiguration Dirac–Hartree–Fock (MCDHF) and relativistic configuration interaction (RCI) methods. With the assistance of the theoretical calculations, eleven observed lines were identified.

2. Experiment

The current experiments were performed in a low-energy electron beam ion trap CUBIT, which has been applied in various measurements of emission lines in highly charged ions [10,14,26]. The operation principle of EBIT has been described in many papers [27,28,29,30,31] in detail. Only a brief description will be given. The CUBIT employs a 0.56 tesla NdFeB permanent magnet to compress the electron beam emitted from a LaB

_{6}

cathode. It usually runs at a few tens of eV to 3 keV, which is sufficient to produce open M-shell ions of medium heavy elements or open N-shell heavy ions. A Wien ion velocity filter is mounted behind the electron collector. The charge state distributions (CSDs) of ions in the trap could be analyzed when extracting the ions in a pulse mode, for unambiguously cataloging the emission lines to the corresponding ions.

The experiment setup was similar to the previous work [14]. In this experiment, the volatile compound Ru(C

_{5}

H

_{5}

)

_{2}

(CAS: 1287-13-4) was continuously injected into the trap region. Ru ions were produced and excited by electron collisions. Light emitted in the decay of the excited ions was focused by a quartz lens mounted outside the vacuum vessel onto the entrance slit of an Andor Shamrock Czerny–Turner spectrometer. The collected light was dispersed by a 1200 mm

^{- 1}

gating and recorded by a charge coupled device. The typical resolving power in the measurement reached about 2700 @427 nm.

A single exposure for one spectrum took two hours, and each line was obtained from the accumulation of at least three exposures to ensure enough statistics and to average out random uncertainties. Line wavelength was calibrated using external Hg, Ar, and Kr lamp reference lines with accurately known wavelength. The validation of the calibration was carefully checked by measuring the emission lines from argon ions with known wavelength.

3. Theoretical Approach

In the present work, the MCDHF and RCI methods were used to calculate the transition energies and transition probabilities. In the MCDHF method, the atomic state function (ASF) is expressed in a linear combination of configuration state functions (CSFs). One of the elaborate tasks in this method is to include the electron correlation effects systematically. The restricted active space method [32,33,34] was used for this purpose.

For Ru

^{24 +}

(3

d^{2}

) and Ru

^{23 +}

(3

d^{3}

), core-valence (CV) correlations were considered by allowing single and double replacements from the

3 d

valance electrons, and single excitation from the

2 s

,

2 p

,

3 s

and

3 p

core subshells to virtual orbitals with

n \leq 7

and

l \leq 5

. The main core-core (CC) correlations were also considered by including double replacements from the

3 p

subshell into the same virtual orbitals. The virtual orbitals were expanded layer by layer. To keep the number of CSFs in a controllable size, for Ru

^{22 +}

(3

d^{4}

) and Ru

^{21 +}

(3

d^{5}

), only the CV correlations from the

3 s

and

3 p

subshells were included. The virtual orbitals were expanded to

n \leq 7

and

l \leq 5

(except

7 h

) for Ru

^{22 +}

(3

d^{4}

), and

n \leq 6

and

l \leq 5

for Ru

^{21 +}

(3

d^{5}

). The numbers of CSFs considered are 853,792, 845,797, 2,230,576 and 595,033 for Ru

^{21 +}

–Ru

^{24 +}

, respectively. The leading QED corrections, namely self-energy and vacuum polarization corrections, and the Breit interaction effect were also included in a followed RCI calculation with the same CSFs described above.

4. Results and Discussion

The nominal electron beam energy varies between 960 eV and 1400 eV to produce the desired ruthenium ions. Due to the complicated charge state distribution evolution in EBIT and the complex atomic structure of the 3d subshell, it is difficult to distinguish the ion abundance simply relying on the electron energy, therefore making it difficult for us to identify emission lines. Spectra observation combing a direct CSDs measurement could solve the dilemma, since in the first approximation the line intensity is proportional to the ion abundance.

We take the Ru

^{23 +}

as an example to introduce the procedure briefly. The charge state distributions of Ru ions along with the line intensity are measured at four electron energies as shown in Figure 1. As illustrated in Figure 1a, the line around 426 nm appears when the electron energy exceeds the ionization threshold of Ru

^{23 +}

. Moreover, the line intensity shows an increasing tendency with the CSDs of Ru

^{23 +}

ions (see Figure 1b). As a result, this line is classified as an emission line from Ru

^{23 +}

ions.

In the same way, spectra of Ru

^{21 +}

–Ru

^{24 +}

ions from 200 to 600 nm are measured, and the wavelengths are determined at the energies in which the abundance of the corresponding ions reach the maximum. In Figure 2, twelve lines in total are observed including four lines from Ru

^{21 +}

, two lines from Ru

^{22 +}

, four lines from Ru

^{23 +}

, and two lines from Ru

^{24 +}

. By comparing with the energies and transition rates calculated with the MCDHF and RCI methods, eleven magnetic dipole lines are identified. As discussed below, the line at 454.730 nm has not been assigned. Experimental and calculated wavelengths (in vacuum) of these transitions are listed in Table 1. The uncertainty (one standard deviation) of each line is listed in the brackets, which consists of three parts, i.e., statistic uncertainties, calibration line uncertainties, and systematic uncertainties caused by the dispersion function. The total uncertainties of these transitions are estimated to be 0.002 to 0.020 nm.

As shown in Table 1, the calculated wavelengths show a good agreement with the experimental results for Ru

^{22 +}

, Ru

^{23 +}

, and Ru

^{24 +}

in general. The deviations are within 1.0% in most cases except for the lines at 338.716 nm and 236.410 nm with the deviation around 2.5%. The deviations of lines from Ru

^{24 +}

are less than 0.3%, which indicates the theoretical model including CV-

2 s 2 p 3 s 3 p

and CC-

3 p

correlations is appropriate. However, we notice that the deviations of lines from Ru

^{21 +}

are as large as 4.5%. Moreover, identification for line at 454.730 nm is still missing. In the Ru

^{21 +}

(3

d^{5}

) calculation, only the CV correlations from

3 s

and

3 p

subshells are included, which may not be adequate to take the main part of correlation effect into account. More complex but efficient theoretical investigations are necessary.

To conclude, twelve lines from Ru

^{21 +}

–Ru

^{24 +}

ions are observed at an EBIT. Eleven of these lines are identified by comparing with theoretical calculation results with the MCDHF-RCI methods, and all of these lines are reported for the first time. The unidentified line at 454.730 nm does not correspond with the calculated results. It is most likely that the half-filled 3d shell of Ru

^{21 +}

requires more consideration of electron correlations. The new measurements provide reference data for further atomic structure studies.

Author Contributions

J.F.: investigation, data curation, writing—original draft, formal analysis; Z.J.: investigation, data curation, writing—original draft, formal analysis; Y.Q.: investigation, formal analysis; J.L. (Jialin Liu): data curation, formal analysis; P.X.: investigation; L.H.: methodology; Z.H.: methodology, formal analysis; Y.Z.: methodology, supervision; J.L. (Jiguang Li): validation, supervision; C.C.: software, validation; and K.Y.: investigation, conceptualization, data curation, funding acquisition, project administration, validation, writing—review and editing. All authors have read and agreed to the published version of the manuscript.

Funding

This work is supported by the National Key Research and Development Program of China under Grant No. 2017YFA0402300, the National Natural Science Foundation of China through Grants No. 11874008.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. (a) Electron beam energy dependence of a transition belonging to Ru

^{23 +}

, (b) the corresponding charge state distributions of ruthenium ions. The relationship between the Wien Filter voltage and the ion charge state was calibrated using argon ions in a pre-experiment. The positions of Ru

^{22 +}

–Ru

^{24 +}

are marked with dashed lines. Two separate peaks are resulted from superposition of peaks of different Ru isotopes.

Figure 1. (a) Electron beam energy dependence of a transition belonging to Ru

^{23 +}

, (b) the corresponding charge state distributions of ruthenium ions. The relationship between the Wien Filter voltage and the ion charge state was calibrated using argon ions in a pre-experiment. The positions of Ru

^{22 +}

–Ru

^{24 +}

are marked with dashed lines. Two separate peaks are resulted from superposition of peaks of different Ru isotopes.

Figure 2. Observed spectra of Ru

^{21 +}

–Ru

^{24 +}

ions. (a) Lines of Ru

^{21 +}

, Ru

^{22 +}

at 1000 and 1100 eV, (b) lines of Ru

^{23 +}

, Ru

^{24 +}

at 1180 and 1400 eV. The lines labeled with arrows represent the transitions with highest intensity from different ions.

Figure 2. Observed spectra of Ru

^{21 +}

–Ru

^{24 +}

ions. (a) Lines of Ru

^{21 +}

, Ru

^{22 +}

at 1000 and 1100 eV, (b) lines of Ru

^{23 +}

, Ru

^{24 +}

at 1180 and 1400 eV. The lines labeled with arrows represent the transitions with highest intensity from different ions.

Table 1. Observed forbidden lines of Ru

^{21 +}

–Ru

^{24 +}

ions. Wavelengths (nm, in vacuum) of experimental and calculated results are listed in the column

λ_{\exp}

and

λ_{theo}

, respectively. The corresponding transitions, transitions rates A, and branch ratios f are also given. The numbers in parentheses denote the uncertainties (one standard deviation), and notation a[b] for transition rates is a ×

10^{b}

. The lable ‘*’ indicates unidentified line.

Table 1. Observed forbidden lines of Ru

^{21 +}

–Ru

^{24 +}

ions. Wavelengths (nm, in vacuum) of experimental and calculated results are listed in the column

λ_{\exp}

and

λ_{theo}

, respectively. The corresponding transitions, transitions rates A, and branch ratios f are also given. The numbers in parentheses denote the uncertainties (one standard deviation), and notation a[b] for transition rates is a ×

10^{b}

. The lable ‘*’ indicates unidentified line.

Ion	Transition	$λ_{\exp}$	$λ_{theo}$	$A (s^{- 1})$	f
Ru $^{21 +}$	${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{7 / 2}$ – ${({(3 d_{3 / 2}^{3})}_{3 / 2} {(3 d_{5 / 2}^{2})}_{4})}_{7 / 2}$	350.662(08)	334.863	1.7[2]	0.30
	${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{7 / 2}$ − ${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{9 / 2}$	420.370(08)	408.831	7.8[1]	0.13
	${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{7 / 2}$ − ${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{5 / 2}$	448.241(05)	430.367	1.8[2]	0.30
	*	454.730(20)
Ru $^{22 +}$	${({(3 d_{3 / 2}^{3})}_{3 / 2} 3 d_{5 / 2}^{1})}_{4}$ − ${(3 d_{3 / 2} {(3 d_{5 / 2}^{3})}_{9 / 2})}_{4}$	248.853(09)	250.803	4.7[2]	0.78
	${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{2})}_{2})}_{1}$ − ${({(3 d_{3 / 2}^{2})}_{2} {(3 d_{5 / 2}^{2})}_{2})}_{0}$	338.716(08)	330.120	4.6[2]	0.11
Ru $^{23 +}$	${(3 d_{3 / 2} {(3 d_{5 / 2}^{2})}_{4})}_{9 / 2}$ − ${({(3 d_{3 / 2}^{2})}_{2} 3 d_{5 / 2})}_{9 / 2}$	236.410(20)	230.532	8.3[2]	0.54
	${(3 d_{3 / 2} {(3 d_{5 / 2}^{2})}_{4})}_{5 / 2}$ − ${({(3 d_{3 / 2}^{2})}_{2} 3 d_{5 / 2})}_{3 / 2}$	255.746(08)	256.305	5.6[2]	0.76
	${({(3 d_{3 / 2}^{2})}_{2} 3 d_{5 / 2})}_{5 / 2}$ − ${(3 d_{3 / 2}^{3})}_{3 / 2}$	426.493(04)	430.663	4.4[2]	1.00
	${(3 d_{3 / 2} {(3 d_{5 / 2}^{2})}_{4})}_{7 / 2}$ − ${({(3 d_{3 / 2}^{2})}_{2} 3 d_{5 / 2})}_{5 / 2}$	504.557(05)	505.204	2.8[2]	1.00
Ru $^{24 +}$	${(3 d_{3 / 2} 3 d_{5 / 2})}_{3}$ − ${(3 d_{3 / 2}^{2})}_{2}$	269.730(02)	270.563	1.1[3]	1.00
	${(3 d_{3 / 2} 3 d_{5 / 2})}_{4}$ − ${(3 d_{3 / 2} 3 d_{5 / 2})}_{3}$	332.755(02)	332.369	4.9[2]	1.00

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Fan, J.; Jiang, Z.; Qian, Y.; Liu, J.; Xu, P.; Huang, L.; He, Z.; Zou, Y.; Li, J.; Chen, C.; et al. Optical Lines of Ru²¹⁺ to Ru²⁴⁺ Ions. Atoms 2022, 10, 154. https://doi.org/10.3390/atoms10040154

AMA Style

Fan J, Jiang Z, Qian Y, Liu J, Xu P, Huang L, He Z, Zou Y, Li J, Chen C, et al. Optical Lines of Ru²¹⁺ to Ru²⁴⁺ Ions. Atoms. 2022; 10(4):154. https://doi.org/10.3390/atoms10040154

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Fan, Junyu, Zihuan Jiang, Yuyuan Qian, Jialin Liu, Pengcheng Xu, Liangyu Huang, Zhencen He, Yaming Zou, Jiguang Li, Chongyang Chen, and et al. 2022. "Optical Lines of Ru²¹⁺ to Ru²⁴⁺ Ions" Atoms 10, no. 4: 154. https://doi.org/10.3390/atoms10040154

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Optical Lines of Ru²¹⁺ to Ru²⁴⁺ Ions

Abstract

1. Introduction

2. Experiment

3. Theoretical Approach

4. Results and Discussion

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Data Availability Statement

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