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177Lu是一种用于成像引导放射性治疗的重要医用同位素, 可通过辐照高丰度176Lu或176Yb的方式生产, 通过同位素分离手段获取高丰度176Lu辐照前体是解决世界范围内177Lu供应不足问题的必要途径 . 由于镥同位素无法通过离心分离方式生产, 需要发展多步多色光电离方法以获取高丰度176Lu, 但镥原子的自电离态能级数据稀缺, 限制了高效光电离路径的构建 . 激光共振电离谱是少数具有自电离态研究能力的激光光谱学方法之一, 利用实验室搭建的激光共振电离飞行时间质谱系统, 测量得到激发态35274.5 cm–1的能级寿命为(31.6 ± 1.7) ns; 由该激发态出发, 利用三色三步光电离方案, 扫描了镥的50560—53450 cm–1能区, 获取了47条自电离态能级, 其中33条为首次发现, 确定了自电离跃迁的峰宽和相对跃迁强度, 提供了可见光波段内可用于镥原子高效光电离的关键光谱数据. 同时, 为确定自电离态能级的电子组态, 通过3条不同J值激发态的扫描实验, 标识了21条能级的角动量, 为确定自其他激发态出发的电偶极跃迁禁戒情况提供了参考依据 .177Lu is an important medical isotope used in imaging-guided radiotherapy, and it can be produced by irradiating 176Lu or 176Yb with high abundance. With an increasing demand for medical isotopes, it is very essential to improve the supply capacity for 177Lu. The multi-step multi-color photoionization method is an effective method to obtain isotopes, and the information of odd-parity autoionization levels is essential. Laser resonance ionization spectroscopy is one of a few spectroscopic experimental methods that can study autoionization levels. An experimental system is developed for the frontier spectroscopic research, and it consists of custom-made tunable lasers and a high-resolution time of flight mass spectrometer. The lifetime of the excited state 35274.5 cm–1 is measured to be (31.6 ± 1.7) ns by the delayed photoionization method for the first time. A three-step three-color photoionization process is used to detect the autoionization levels, with a delay of 30 ns between λ2 – λ1 and λ3 – λ2 respectively, in order to avoid any unexpected transitions. Forty-seven odd-parity autoionization levels are obtained, of which 33 levels are discovered for the first time, and the λ2 and λ1 are blocked to exclude possible interference peaks, such as the λ1+λ3+λ3 transition. Several autoionization levels show asymmetrical peak shapes, and the Fano fitting is carried out for all the levels to determine the widths and relative transition strengths of the autoionizing transitions. This study provides critical data for the high-efficient photoionization of lutetium atoms in the visible range. The angular momenta of 21 odd-parity autoionization levels in an energy range of 50650–51650 cm–1 are identified for the first time, which provides a reference for determining the forbidden state of electric dipole transitions from other excited states and ascertaining the electronic configuration.
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Keywords:
- autoionization levels /
- resonance ionization /
- lutetium atom
[1] Fuoco V, Argiroffi G, Mazzaglia S, Lorenzoni A, Guadalupi V, Franza A, Scalorbi F, Ailberti G, Chiesa C, Procopio G, Seregni E, Maccauro M 2022 Tumori. J. 108 315
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图 1 激光共振电离飞行时间质谱系统. PC为电脑, DG为延时发生器, Nd:YAG为Nd:YAG激光器, Dye为染料激光器, WM为波长计, BS为光束合成器, Lens为镜组, ECB为电控机箱, TOF为飞行时间质谱, BCA为Boxcar平均
Fig. 1. Resonance ionization time-of-flight mass spectroscopy system. PC is computer, DG is delay generator, Nd:YAG is Nd:YAG laser, Dye is dye laser, WM is wavelength meter, BS is beam synthesis, Lens is lens, ECB is electronic control box, TOF is time of flight mass spectrometry, BCA is box car averager.
图 2 多步多色光电离路径示意图
Fig. 2. Schematic representation of the multi-step multi-color photoionization path.
表 1 由激发态35274.5 cm–1跃迁的奇宇称自电离态能级
Table 1. Odd parity autoionization levels connecting from the excited level 35274.5 cm–1.
E/cm–1 Width Strength Ref.[18] E/cm–1 Width Strength Ref.[18] 53408.90 N S New 51873.82 B I New 53353.74 Ϯ B S New 51724.60 Ϯ M S New 53330.68 M I New 51642.24 N S 51642.2 53321.80 N I New 51628.73 N I 51628.9 53310.02 M S New 51509.40 M S 51509.4 53298.32 N I New 51494.64 B S New 53267.79 M S New 51368.06 M S 51386.0 53259.85 N W New 51295.65 Ϯ B W 51294.1 53251.30 N I New 51150.11 Ϯ B W 51151.5 53219.59 Ϯ M S New 51125.54 B I New 53194.18 Ϯ B I New 51014.87 M W New 53147.77 M W New 50986.87 N W 50987.0 53138.94 Ϯ M I New 50974.56 N W 50974.7 53046.75 Ϯ B I New 50950.65 M I 50950.7 53033.60 Ϯ M I New 50908.68 Ϯ B I New 52981.68 Ϯ B I New 50875.33 M W 50875.1 52806.85 M I New 50872.30 M I 50872.3 52678.69 Ϯϯ B S New 50834.41 Ϯ B I 50833.3 52490.86 Ϯ B W New 50804.68 N W New 52420.31 N W New 50774.92 Ϯ M I 50774.3 52415.04 N W New 50726.72 Ϯ M S New 52377.33 Ϯ M I New 50700.60 M S 50700.7 52280.25 N I New 50657.49 M S 50657.6 52508.75 B W New — — — — 注: Ϯ 谱线呈现Fano峰形; ϯ 极宽峰, 峰半高宽＞100 cm–1. 
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表 2 奇宇称自电离态能级的角动量
Table 2. J-values of odd parity autoionization levels.
From 35274.5 cm–1 From 33831.5 cm–1 [18] From 34610.5 cm–1 J E/cm–1 Width E/cm–1 Width E/cm–1 Width 51642.21 N 51642.2 N 51642.06 N 3/2 51628.71 N 51628.9 N 51629.03 N 3/2 51509.42 M 51509.4 N — — 5/2 51494.66 B — — — — 7/2 51368.06 M 51368.0 N 51368.12 M 3/2 51295.65 B 51294.1 B — — 5/2 51014.87 B — — — — 7/2 50986.87 N 50987.0 N — — 5/2 50974.56 N 50974.7 N 50974.47 M 3/2 50950.65 M 50950.7 N — — 5/2 — — 50913.3 N 50913.18 N 1/2 50908.68 B — — — — 7/2 — — 50887.8 N 50887.65 N 1/2 50875.33 M 50875.1 B 50875.32 M 3/2 50872.30 M 50872.3 N — — 5/2 50834.41 B 50833.3 B 50832.77 B 3/2 50804.68 N — — — — 7/2 50774.92 M 50774.3 M 50773.31 M 3/2 50726.72 M — — — — 7/2 50700.60 M 50700.7 N — — 5/2 50657.49 M 50657.6 N — — 5/2
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[1] Fuoco V, Argiroffi G, Mazzaglia S, Lorenzoni A, Guadalupi V, Franza A, Scalorbi F, Ailberti G, Chiesa C, Procopio G, Seregni E, Maccauro M 2022 Tumori. J. 108 315
Google Scholar
[2] Mittra E S 2018 Am. J. Roentgenol. 211 278
Google Scholar
[3] Vogel W V, van der Marck S C, Versleijen M W J 2021 Eur. J. Nucl. Med. Mol. I. 48 2329
Google Scholar
[4] Dash A, Pillai M R A, Knapp F F 2015 Nucl. Med. Molec. Imag. 49 85
Google Scholar
[5] D’yachkov A B, Kovalevich S K, Labozin A V, Labozin V P, Mironov S M, Panchenko V Y, Firsov V A, Tsvetkov G O, Shatalova G G 2012 Quantum Electron 42 953
Google Scholar
[6] Gadelshin V, Cocolios T, Fedoseev V, Heinke R, Kieck T, Marsh B, Naubereit P, Rothe S, Stora T, Studer D, van Duppen P, Wendt K 2017 HFI 238 28
Google Scholar
[7] Li R, Lassen J, Kunz P, Mostamand M, Reich B B, Teigelhofer A, Yan H, Ames F 2019 Spectrochim. Acta B 158 105633
Google Scholar
[8] Gadelshin V, Heinke R, Kieck T, Kron T, Naubereit P, Rosch F, Stora T, Studer D, Wendt K 2019 Radiochim. Acta 107 653
Google Scholar
[9] Suryanarayana M V, Sankari M 2021 Sci. Rep-UK 11 18292
Google Scholar
[10] Suryanarayana M V 2021 Sci. Rep-UK 11 6118
Google Scholar
[11] Wendt K, Trautmann N 2005 Int. J. Mass. Spectrom. 242 161
Google Scholar
[12] Xu C B, Xu X Y, Ma H, Li L Q, Huang W, Chen D Y, Zhu F R 1993 J. Phys. B-At. Mol. Opt. 26 2827
Google Scholar
[13] Kujirai O, Ogawa Y 1998 J. Phys. Soc. Jpn. 63 1056
Google Scholar
[14] Ogawa Y, Kujirai O 1999 J. Phys. Soc. Jpn. 68 428
Google Scholar
[15] Li R, Lassen J, Zhong Z P, Jia F D, Mostamand M, Li X K, Reich B B, Teigelhofer A, Yan H 2017 Phys. Rev. A 95 052501
Google Scholar
[16] 李志明, 朱凤蓉, 张子斌, 邓虎, 翟利华, 王长海, 任向军, 万可友, 张利兴 2005 质谱学报 26 45
Google Scholar
Li Z M, Zhu F R, Zhang Z B, Deng H, Zhai L H, Wang C H, Ren X J, Wan K Y, Zhang L X 2005 J. Chin. Mass. Spectr. Soc. 26 45
Google Scholar
[17] D’yachkov A B, Gorkunov A A, Labozin A V, Mironov S M, Tsvetkov G O, Panchenko V Y, Firsov V A 2018 Opt. Spectrosc 125 839
Google Scholar
[18] Rath A D, Biswal D, Kundu S 2021 J. Quant. Spectrosc. Ra. 270 107696
Google Scholar
[19] Voss A, Sonnenschein V, Campbell P, Cheal B, Kron T, Moore I D, Pohjalainen I, Raeder S, Trautmann N, Wendt K 2017 Phys. Rev. A 95 032506
Google Scholar
[20] Shen X P, Wang W L, Zhai L H, Deng H, Xu J, Yuan X L, Wei G Y, Wang W, Fang S, Su Y Y, Li Z M 2018 Spectrochim. Acta B 145 96
Google Scholar
[21] Kneip N, Dullmann C E, Gadelshin V, Heinke R, Mokry C, Raeder S, Runke J, Studer D, Trautmann N, Weber F, Wendt K 2020 HFI 241 45
Google Scholar
[22] Sahoo A C, Mandal P K, Shah M L, Dev V 2020 J. Quant. Spectrosc. Ra. 241 106714
Google Scholar
[23] 张钧尧, 薛轶, 周鸿儒 2024 原子与分子 41 014002
Google Scholar
Zhang J Y, Xue Y, Zhou H R 2024 J. Atom. Mol. Phys. 41 014002
Google Scholar
[24] 李云飞, 张钧尧, 柴俊杰, 魏少强, 陈晨 2023 真空与低温 29 486
Google Scholar
Li Y F, Zhang J Y, Chai J J, Wei S Q, Chen C 2023 Vacuum and Cryogenics 29 486
Google Scholar
[25] Fedchak J A, der Hartog E A, Lawler J E, Palmeri P, Quinet P, Biemont E 2000 Astrophys. J. 542 1109
Google Scholar
[26] Fano U 1961 Phys. Rev. 124 1866
Google Scholar
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