惰性气体Rydberg态和自电离态光谱研究
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摘要
原子高激发态的研究在天体物理、受控核聚变、电子关联效应、激光分离同位素,以及新型激光器的研制等领域有着重要的意义。本论文主要报道惰性气体原子自电离态的光激发谱研究。我们采用脉冲直流放电和超声射流冷却相结合的方法产生惰性气体亚稳态,利用光激发和时间飞行质谱技术,研究了Ar,Kr,Xe三种惰性气体自电离态激发谱。本论文主要从:Ar原子自电离Rydberg态光谱研究,Kr原子自电离Rydberg态光谱研究,Xe原子自电离Rydberg态光谱研究三个部分进行了讨论。
实验中我们采用气体脉冲直流放电的方法,产生分别位于93143.767cm~(-1)和94553.67 cm~(-1)处的亚稳态Ar~*(3p~54s[3/2]_2和3p~54s′[1/2]_0),分别位于79971.7321cm~(-1)和85191.6075 cm~(-1)处的亚稳态Kr~*(4p~55s[3/2]_2和4p~55s′[1/2]_0),以及分别位于67067.54cm~(-1)和76196.78 cm~(-1)处的亚稳态Xe~*(5p~56s[3/2]_2和5p~56s′[1/2]_0)。随后用脉冲紫外激光单光子激发其到偶宇称自电离共振态序列np′[3/2]_(1,2),[1/2]_1,nf′[5/2]_3。通过时间飞行质谱(TOF—MS)技术收集自电离所得Ar,Kr,Xe离子得到235—358 nm激光波长范围内自电离共振态的激发谱,光谱分辨～0.1 cm~(-1)。主要完成以下工作:
(1)系统地观测到了Ar原子3p~5(~2P_(1/2))np′[3/2]_2(n=11-39),[3/2]_1(n=11-29),[1/2]_1(n=11-22)和3p~5(~2P_(1/2))nf′[5/2]_3(n=9-38)Rydberg序列自电离态,Kr原子4p~5(~2P_(1/2))np′[3/2]_2(n=8-39),[3/2]_1(n=8-34),[1/2]_1(n=8-26)和3p~5(~2P_(1/2))nf′[5/2]_3(n=5-34)Rydberg序列自电离态,和Xe原子5p~5(~2P_(1/2))np′[3/2]_1(n=7-28),[1/2]_1(n=7-37)和5p~5(~2P_(1/2))nf′[5/2]_3(n=4-31)Rydberg序列自电离态基于其亚稳态单光子跃迁的激发谱,通过分析光谱得到这些自电离态的能级与量子亏损数据,由此确定了自电离态更完整和精确的光谱数据,其中部分数据为首次获得;
(2)对Ar原子3p~5(~2P_(1/2))np′和3p~5(~2P_(1/2))nf′序列,Kr原子4p~5(~2P_(1/2))np′和4p~5(~2P_(1/2))nf′序列以及Xe原子5p~5(~2P_(1/2))np′和5p~5(~2P_(1/2))nf′序列Rydberg自电离态的激发谱进行分析,确定其不对称光谱线形属于自电离共振态与连续态相互作用产生的Fano线形,首次系统地对Ar,Kr,Xe原子自电离态激发谱进行拟合得到系列的自电离共振态的能级位置,量子亏损δ,Fano线形因子q,共振宽度Γ,共振态寿命τ和衰减宽度Γ_r等参数。其中q,Γ和τ与有效量子数n~*直接相关。
(3)根据对激发谱的数据分析得到Ar原子的3p~5np′Rydberg序列[3/2]_2,[3/2]_1和[1/2]_1自电离态的能级间距,Kr原子的4p~5np′Rydberg序列[3/2]_2,[3/2]_1和[1/2]_1自电离态的能级间距,以及Xe原子的5p~5np′Rydberg序列[3/2]_1和[1/2]_1自电离态的能级间距,根据精细结构间距的理论对之进行分析,与理论预测相符。
(4)观测到高分辨的无微扰的Ar原子3p~5nf′(n=13,14,15)序列,Kr原子4p~5nf′(n=13,14,15,16,17)序列,以及Xe原子5p~5nf′(n=11,12,13,14,15)序列在不同外电场强度条件下的Stark分裂光谱,根据简并微扰理论对其进行了分析。
(5)观测到清晰的Ar,Kr,Xe原子第一电离限~2P_(3/2)在不同外电场条件下的偏移,对其进行了合理的解释。
The atom spectroscopy on atom high-excited states is of great significance in many fields such as astrophysics,controlled nuclear fusion,electron correlation effects, laser isotope separation,and new laser system developing,and so on.This dissertation presents the experimental study on excitation spectra of rare gas autoionizing resonances.The metastable levels of the rare gases were produced by the pulsed DC discharge under the supersonic free jet condition and investigated by laser excitation spectroscopy and time-of-flight ion detection.This dissertation contains three parts: the autoionizing resonances and Rydberg states spectrum of Ar;the autoionizing resonances and Rydberg states spectrum of Kr;the autoionizing resonances and Rydberg states spectrum of Xe.
Metastable Ar~*,Kr~* and Xe~* atoms were produced in their metastable states mp~5(m+1)s[3/2]_2 and mp~5(m+1)s'[1/2]_0(m=3,4,5 for Ar,Kr and Xe respectively)by a pulsed DC discharge in a beam,and were subsequently excited to the even-parity autoionizing resonance series mp~5np'[3/2]_(1,2),mp~5np'[1/2]_1,and mp~5nf[5/2]_3(m= 3,4,5 for Ar,Kr and Xe respectively)by single photon excitation with a pulsed dye laser.The excitation spectra of the even-parity autoionizing resonance series from the metastable Ar~*,Kr~* and Xe~* were obtained by recording the Ar~+,Kr~+ and Xe~+ ions with MCP detection on time-of-flight in the photon energy range of 28000-40000 cm~(-1)with an experimental bandwidth of～0.1cm~(-1).The main results are summarized as follows:
(1)The series levels and quantum defects of rare gases autoionizing resonances are determined:for Ar autoionizing resonances states 3p~5(~2P_(1/2))np'[3/2]_2(n=11-39), [3/2]_1(n=11-29),[1/2]_1(n=11-22),3p~5(~2P_(1/2))nf'[5/2]_3(n=9-38);for Kr autoionizing resonances states 4p~5(~2P_(1/2))np'[3/2]_2(n=8-39),[3/2]_1(n=8-34),[1/2]_1 (n=8-26),4p~5(~2P_(1/2))nf[5/2]_3(n=5-34);for Xe autoionizing resonances states 5p~5(~2P_(1/2))np'[3/2]_1(n=7-28),[1/2]_1(n=7-37),5p~5(~2P_(1/2))nf[5/2]_3(n=4-31). Almost half of the data is reported firstly.
(2)Quantum defects,line profile index and resonance widths,resonance lifetime and reduced widths of the autoionizing resonances states were derived by a Fano-type line-shape analysis for all observed levels which most of them were observed first time in current operation.The line profile index q and the resonance widthsΓare shown to be approximately proportional to the effective principal quantum number n~*.
(3)The line separation of the mp~5np'(m=3,4,5 for Ar,Kr and Xe respectively) autoionizing resonances was observed and discussed.
(4)The high resolution Stark effect spectroscopy of mp~5nf'(m=3,4,5 for Ar,Kr and Xe respectively)autoionizing resonances in various electric field strengths were detected,and discussed with degenerate perturbation theory.The experiment results accord with the theory very well.
(5)The shifts of the ionization potential in various electric field strengths were discussed at last.
实验中我们采用气体脉冲直流放电的方法,产生分别位于93143.767cm~(-1)和94553.67 cm~(-1)处的亚稳态Ar~*(3p~54s[3/2]_2和3p~54s′[1/2]_0),分别位于79971.7321cm~(-1)和85191.6075 cm~(-1)处的亚稳态Kr~*(4p~55s[3/2]_2和4p~55s′[1/2]_0),以及分别位于67067.54cm~(-1)和76196.78 cm~(-1)处的亚稳态Xe~*(5p~56s[3/2]_2和5p~56s′[1/2]_0)。随后用脉冲紫外激光单光子激发其到偶宇称自电离共振态序列np′[3/2]_(1,2),[1/2]_1,nf′[5/2]_3。通过时间飞行质谱(TOF—MS)技术收集自电离所得Ar,Kr,Xe离子得到235—358 nm激光波长范围内自电离共振态的激发谱,光谱分辨～0.1 cm~(-1)。主要完成以下工作:
(1)系统地观测到了Ar原子3p~5(~2P_(1/2))np′[3/2]_2(n=11-39),[3/2]_1(n=11-29),[1/2]_1(n=11-22)和3p~5(~2P_(1/2))nf′[5/2]_3(n=9-38)Rydberg序列自电离态,Kr原子4p~5(~2P_(1/2))np′[3/2]_2(n=8-39),[3/2]_1(n=8-34),[1/2]_1(n=8-26)和3p~5(~2P_(1/2))nf′[5/2]_3(n=5-34)Rydberg序列自电离态,和Xe原子5p~5(~2P_(1/2))np′[3/2]_1(n=7-28),[1/2]_1(n=7-37)和5p~5(~2P_(1/2))nf′[5/2]_3(n=4-31)Rydberg序列自电离态基于其亚稳态单光子跃迁的激发谱,通过分析光谱得到这些自电离态的能级与量子亏损数据,由此确定了自电离态更完整和精确的光谱数据,其中部分数据为首次获得;
(2)对Ar原子3p~5(~2P_(1/2))np′和3p~5(~2P_(1/2))nf′序列,Kr原子4p~5(~2P_(1/2))np′和4p~5(~2P_(1/2))nf′序列以及Xe原子5p~5(~2P_(1/2))np′和5p~5(~2P_(1/2))nf′序列Rydberg自电离态的激发谱进行分析,确定其不对称光谱线形属于自电离共振态与连续态相互作用产生的Fano线形,首次系统地对Ar,Kr,Xe原子自电离态激发谱进行拟合得到系列的自电离共振态的能级位置,量子亏损δ,Fano线形因子q,共振宽度Γ,共振态寿命τ和衰减宽度Γ_r等参数。其中q,Γ和τ与有效量子数n~*直接相关。
(3)根据对激发谱的数据分析得到Ar原子的3p~5np′Rydberg序列[3/2]_2,[3/2]_1和[1/2]_1自电离态的能级间距,Kr原子的4p~5np′Rydberg序列[3/2]_2,[3/2]_1和[1/2]_1自电离态的能级间距,以及Xe原子的5p~5np′Rydberg序列[3/2]_1和[1/2]_1自电离态的能级间距,根据精细结构间距的理论对之进行分析,与理论预测相符。
(4)观测到高分辨的无微扰的Ar原子3p~5nf′(n=13,14,15)序列,Kr原子4p~5nf′(n=13,14,15,16,17)序列,以及Xe原子5p~5nf′(n=11,12,13,14,15)序列在不同外电场强度条件下的Stark分裂光谱,根据简并微扰理论对其进行了分析。
(5)观测到清晰的Ar,Kr,Xe原子第一电离限~2P_(3/2)在不同外电场条件下的偏移,对其进行了合理的解释。
The atom spectroscopy on atom high-excited states is of great significance in many fields such as astrophysics,controlled nuclear fusion,electron correlation effects, laser isotope separation,and new laser system developing,and so on.This dissertation presents the experimental study on excitation spectra of rare gas autoionizing resonances.The metastable levels of the rare gases were produced by the pulsed DC discharge under the supersonic free jet condition and investigated by laser excitation spectroscopy and time-of-flight ion detection.This dissertation contains three parts: the autoionizing resonances and Rydberg states spectrum of Ar;the autoionizing resonances and Rydberg states spectrum of Kr;the autoionizing resonances and Rydberg states spectrum of Xe.
Metastable Ar~*,Kr~* and Xe~* atoms were produced in their metastable states mp~5(m+1)s[3/2]_2 and mp~5(m+1)s'[1/2]_0(m=3,4,5 for Ar,Kr and Xe respectively)by a pulsed DC discharge in a beam,and were subsequently excited to the even-parity autoionizing resonance series mp~5np'[3/2]_(1,2),mp~5np'[1/2]_1,and mp~5nf[5/2]_3(m= 3,4,5 for Ar,Kr and Xe respectively)by single photon excitation with a pulsed dye laser.The excitation spectra of the even-parity autoionizing resonance series from the metastable Ar~*,Kr~* and Xe~* were obtained by recording the Ar~+,Kr~+ and Xe~+ ions with MCP detection on time-of-flight in the photon energy range of 28000-40000 cm~(-1)with an experimental bandwidth of～0.1cm~(-1).The main results are summarized as follows:
(1)The series levels and quantum defects of rare gases autoionizing resonances are determined:for Ar autoionizing resonances states 3p~5(~2P_(1/2))np'[3/2]_2(n=11-39), [3/2]_1(n=11-29),[1/2]_1(n=11-22),3p~5(~2P_(1/2))nf'[5/2]_3(n=9-38);for Kr autoionizing resonances states 4p~5(~2P_(1/2))np'[3/2]_2(n=8-39),[3/2]_1(n=8-34),[1/2]_1 (n=8-26),4p~5(~2P_(1/2))nf[5/2]_3(n=5-34);for Xe autoionizing resonances states 5p~5(~2P_(1/2))np'[3/2]_1(n=7-28),[1/2]_1(n=7-37),5p~5(~2P_(1/2))nf[5/2]_3(n=4-31). Almost half of the data is reported firstly.
(2)Quantum defects,line profile index and resonance widths,resonance lifetime and reduced widths of the autoionizing resonances states were derived by a Fano-type line-shape analysis for all observed levels which most of them were observed first time in current operation.The line profile index q and the resonance widthsΓare shown to be approximately proportional to the effective principal quantum number n~*.
(3)The line separation of the mp~5np'(m=3,4,5 for Ar,Kr and Xe respectively) autoionizing resonances was observed and discussed.
(4)The high resolution Stark effect spectroscopy of mp~5nf'(m=3,4,5 for Ar,Kr and Xe respectively)autoionizing resonances in various electric field strengths were detected,and discussed with degenerate perturbation theory.The experiment results accord with the theory very well.
(5)The shifts of the ionization potential in various electric field strengths were discussed at last.
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