飞秒激光诱导等离子体光谱时空特性的研究
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摘要
在过去二十多年的时间里,关于利用飞秒激光诱导等离子体发射光谱来研究激光等离子体的基本特性的研究一直持续着,由于飞秒激光特有的时间特性,从而使得飞秒激光诱导等离子体具有着特殊的时空特性,本文的工作由此展开。
1、首次对空气中飞秒激光诱导等离子体光谱的角分布特性进行了研究,发现正一价氮气分子的391.5nm谱线和氮原子的744.2nm谱线存在着不同的角分布。两条谱线存在类似的变化趋势,通过偶极子辐射的角分布特性和诱导形成的等离子体的荧光的分布建立了计算模型,并与实验结果符合的很好。随后根据实验结果和计算结果的对比,得到了氮气分子与原子的极化度随等离子体通道位置的关系曲线,发现在空气等离子体中氮气分子的极化度大于氮原子极化度,两者存在类似的变化趋势的同时又存在着明显的差异,其原因在于空气中的氮原子或者离子都是由激光电离激发后的氮气分子解离而来,且解离后的原子或离子的初始动量存在特有的角分布。
2、首次对飞秒脉冲激光在不同配比,不同气压下(低于一个标准大气压)的氮气与氩气的混合气体中,等离子体光谱的时间演化特性进行了研究。实验结果表明氮气分子谱线与氮离子谱线光谱的持续时间都在20ns左右,且有着不同的气压特性,其中氮离子谱线只出现在气压低于6的情况下,气压大于10kPa时,氮气分子谱线才会出现,并随着气压的增大,谱线强度也在增大。而正一价氮气谱线却存在于整个实验中的气压测量范围内。利用氮离子谱线计算了不同配比的气体中等离子体温度和电子密度随时间的变化曲线,发现等离子体的温度会在10ns时间内快速上升,然后保持在7000K左右,且不会随氩气配比的增加而变化。气压从1kPa增加到6kPa时,等离子体的电子密度是增加的；在时间方面,气压不变的情况下,电子密度迅速达到最大,随后缓慢的降低。随着氮气中氩气含量的增加,在1kPa和2kPa时,电子密度会减小,但是当气压为4kPa和6kPa时,则有着相反的变化趋势。在大于10kPa时,氮气分子谱线会随着随氩气配比的增加而增加。
三、分别对低于一个标准大气压的空气和氩气的环境气体条件下的飞秒激光诱导镍等离子体光谱进行了实验研究。结果表明,在两种环境气体中,镍等离子体光谱均表现为连续谱和原子线状谱的叠加。随着环境气压的降低,由于电子密度的下降,从而使得低压条件下的谱线比高压条件下的潜线具有更好的分辨。同时,谱线强度经历了由缓慢增强发展到迅速降低的演化过程。另外,论文还讨论了环境气体成分对谱线强度的影响。
以上的研究成果有利于人们更深入地理解飞秒脉冲激光诱导等离子体的基本特性及其变化情况。对目前飞秒脉冲激光的发展和应用提供了有益的支持。
In the last20years, the study of the characteristics of the laser-induced plasma has been always carried out intensively by the femtosecond laser-induced breakdown spectroscopy (LIBS) technique. Due to the time characteristics of femtosecond laser pulse, the femtosecond laser-induced plasma emission spectroscopy has special spatiotemporal characteristics. That is the initial motivation of this paper.
First, For the first time, the angular distribution of femtosecond laser-induced plasma emission spectroscopy involving pulse filamentation in air was experimentally and theoretically investigated. The391.5nm spectral line of N2+and744.2nm spectral line of N2have similar angular distribution behaviors. By using the angular distribution of dipole radiation and laser-induced plasma fluorescence distribution, we build up an analysis model to calculate the the angular distribution of femtosecond laser-induced plasma emission spectroscopy, which is in good agreement with the experimental results. Then, based on the comparison of experimental data and the calculated one, the polarization of the nitrogen molecules and atoms as a function of the position of plasma channel was derived. In the plasma generated during pulse filamentation, the polarization of nitrogen molecules is larger than that of nitrogen atoms. There are similar polarization trend between nitrogen molecules and nitrogen atoms but with obvious difference, because the nitrogen atoms are all from the dissociation of nitrogen molecules and they initial momentum has certain angular distribution.
Second:Study of temporal characterization of femtosecond pulse laser induced spectroscopy in five kinds of mixed gas with different pressure (Less than a standard atmospheric pressure). The time-domain evolution of plasma spectroscopy was experimentally investigated in different ratio of nitrogen with argon in different gas pressures. The results show that the decay time of spectral lines of nitrogen molecules and nitrogen ions are approximate20ns. The spectral lines of N+only appear under6kPa and the spectral lines of N2are absent when the pressures are lower than10kPa. The intensity of spectral lines of N2is increased with rising of gas pressure. However, the spectral lines of N2+exist during the whole pressure region. Then we calculated the plasma density and temperature as a function of time by using the spectra of NII. The plasma temperature rapidly goes up during10ns and then remains a constant of about7000K, which does not change with the ratio of argon. The plasma density increases when the pressure changes from1kPa to6kPa. In the time domain under certain pressure, the plasma density reaches the maximum and then gradually decays. With the increasing ratio of Ar, the plasma density decreases under pressure of1kPa and2kPa, but reverse under pressure of4kPa and6kPa. When the pressure is larger than lOkPa, the intensity of spectral lines of N2is increased with the increasing ratio of argon.
Third, The spectra of Ni plasma induced by femtosecond laser pulses at sub-atmospheric pressure environment has been studied experimentally in air and argon gas, respectively. The results show that the spectra of laser-induced plasmas are composed of continuous spectra and atomic line spectra in these two surrounding gases. With the reduction of surrounding gas pressure, the spectra at lower surrounding pressure show higher resolution due to the decrease of electron density, compared to that at higher pressure. Besides, the intensity of line spectra undergoes the transition from slow increase to rapid decrease. Additionally, the effect of the composition of the surrounding gas on the intensity is also briefly discussed in this paper.
The research results presented in this dissertation are useful for further understanding of the characteristics of femtosecond laser-induced plasma emission spectroscopy, and give support for application of femtosecond laser.
1、首次对空气中飞秒激光诱导等离子体光谱的角分布特性进行了研究,发现正一价氮气分子的391.5nm谱线和氮原子的744.2nm谱线存在着不同的角分布。两条谱线存在类似的变化趋势,通过偶极子辐射的角分布特性和诱导形成的等离子体的荧光的分布建立了计算模型,并与实验结果符合的很好。随后根据实验结果和计算结果的对比,得到了氮气分子与原子的极化度随等离子体通道位置的关系曲线,发现在空气等离子体中氮气分子的极化度大于氮原子极化度,两者存在类似的变化趋势的同时又存在着明显的差异,其原因在于空气中的氮原子或者离子都是由激光电离激发后的氮气分子解离而来,且解离后的原子或离子的初始动量存在特有的角分布。
2、首次对飞秒脉冲激光在不同配比,不同气压下(低于一个标准大气压)的氮气与氩气的混合气体中,等离子体光谱的时间演化特性进行了研究。实验结果表明氮气分子谱线与氮离子谱线光谱的持续时间都在20ns左右,且有着不同的气压特性,其中氮离子谱线只出现在气压低于6的情况下,气压大于10kPa时,氮气分子谱线才会出现,并随着气压的增大,谱线强度也在增大。而正一价氮气谱线却存在于整个实验中的气压测量范围内。利用氮离子谱线计算了不同配比的气体中等离子体温度和电子密度随时间的变化曲线,发现等离子体的温度会在10ns时间内快速上升,然后保持在7000K左右,且不会随氩气配比的增加而变化。气压从1kPa增加到6kPa时,等离子体的电子密度是增加的；在时间方面,气压不变的情况下,电子密度迅速达到最大,随后缓慢的降低。随着氮气中氩气含量的增加,在1kPa和2kPa时,电子密度会减小,但是当气压为4kPa和6kPa时,则有着相反的变化趋势。在大于10kPa时,氮气分子谱线会随着随氩气配比的增加而增加。
三、分别对低于一个标准大气压的空气和氩气的环境气体条件下的飞秒激光诱导镍等离子体光谱进行了实验研究。结果表明,在两种环境气体中,镍等离子体光谱均表现为连续谱和原子线状谱的叠加。随着环境气压的降低,由于电子密度的下降,从而使得低压条件下的谱线比高压条件下的潜线具有更好的分辨。同时,谱线强度经历了由缓慢增强发展到迅速降低的演化过程。另外,论文还讨论了环境气体成分对谱线强度的影响。
以上的研究成果有利于人们更深入地理解飞秒脉冲激光诱导等离子体的基本特性及其变化情况。对目前飞秒脉冲激光的发展和应用提供了有益的支持。
In the last20years, the study of the characteristics of the laser-induced plasma has been always carried out intensively by the femtosecond laser-induced breakdown spectroscopy (LIBS) technique. Due to the time characteristics of femtosecond laser pulse, the femtosecond laser-induced plasma emission spectroscopy has special spatiotemporal characteristics. That is the initial motivation of this paper.
First, For the first time, the angular distribution of femtosecond laser-induced plasma emission spectroscopy involving pulse filamentation in air was experimentally and theoretically investigated. The391.5nm spectral line of N2+and744.2nm spectral line of N2have similar angular distribution behaviors. By using the angular distribution of dipole radiation and laser-induced plasma fluorescence distribution, we build up an analysis model to calculate the the angular distribution of femtosecond laser-induced plasma emission spectroscopy, which is in good agreement with the experimental results. Then, based on the comparison of experimental data and the calculated one, the polarization of the nitrogen molecules and atoms as a function of the position of plasma channel was derived. In the plasma generated during pulse filamentation, the polarization of nitrogen molecules is larger than that of nitrogen atoms. There are similar polarization trend between nitrogen molecules and nitrogen atoms but with obvious difference, because the nitrogen atoms are all from the dissociation of nitrogen molecules and they initial momentum has certain angular distribution.
Second:Study of temporal characterization of femtosecond pulse laser induced spectroscopy in five kinds of mixed gas with different pressure (Less than a standard atmospheric pressure). The time-domain evolution of plasma spectroscopy was experimentally investigated in different ratio of nitrogen with argon in different gas pressures. The results show that the decay time of spectral lines of nitrogen molecules and nitrogen ions are approximate20ns. The spectral lines of N+only appear under6kPa and the spectral lines of N2are absent when the pressures are lower than10kPa. The intensity of spectral lines of N2is increased with rising of gas pressure. However, the spectral lines of N2+exist during the whole pressure region. Then we calculated the plasma density and temperature as a function of time by using the spectra of NII. The plasma temperature rapidly goes up during10ns and then remains a constant of about7000K, which does not change with the ratio of argon. The plasma density increases when the pressure changes from1kPa to6kPa. In the time domain under certain pressure, the plasma density reaches the maximum and then gradually decays. With the increasing ratio of Ar, the plasma density decreases under pressure of1kPa and2kPa, but reverse under pressure of4kPa and6kPa. When the pressure is larger than lOkPa, the intensity of spectral lines of N2is increased with the increasing ratio of argon.
Third, The spectra of Ni plasma induced by femtosecond laser pulses at sub-atmospheric pressure environment has been studied experimentally in air and argon gas, respectively. The results show that the spectra of laser-induced plasmas are composed of continuous spectra and atomic line spectra in these two surrounding gases. With the reduction of surrounding gas pressure, the spectra at lower surrounding pressure show higher resolution due to the decrease of electron density, compared to that at higher pressure. Besides, the intensity of line spectra undergoes the transition from slow increase to rapid decrease. Additionally, the effect of the composition of the surrounding gas on the intensity is also briefly discussed in this paper.
The research results presented in this dissertation are useful for further understanding of the characteristics of femtosecond laser-induced plasma emission spectroscopy, and give support for application of femtosecond laser.
引文
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