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摘要:
激光诱导击穿光谱技术(Laser-Induced Breakdown Spectroscopy，LIBS)是利用强脉冲激光与物质相互作用所产生的等离子体光谱来实现对物质组成元素定性和定量分析的一种新方法。在脉冲激光诱导等离子体的过程中，不同的激光参数(能量、脉宽、波长)、检测过程中的环境条件以及材料本身的特性等，对激光诱导等离子体的物理机制都有不同程度的影响，进而影响LIBS定量分析的结果。本文综述了现阶段LIBS技术中涉及的物理机制，包括LIBS基本原理、激光参数区别、环境和材料特性差异所涉及的物理机制。为深入理解激光与物质相互作用、提升LIBS检测能力提供了依据。
- 激光诱导击穿光谱(LIBS) /
- 原理 /
- 物理机制
Abstract:
Laser Induced Breakdown Spectroscopy (LIBS) is a new method for qualitative and quantitative analysis of the constituents of a material using plasma spectra produced by the interaction of a strong pulsed laser with the material. In the process of pulsed laser-induced plasma, different laser parameters (energy, pulse width, wavelength), environmental conditions during the detection process and the properties of the material itself have varying degrees of influence on the physical mechanism of laser-induced plasma, which in turn affects the results of LIBS quantitative analysis. This paper reviews the physical mechanisms involved in the current state of LIBS technology, including the basic principles of LIBS, the differences in laser parameters, and the physical mechanisms involved in the differences in environmental and material properties. It provides a basis for a deeper understanding of laser-matter interactions and for improving the detection capabilities of LIBS.
- Laser Induced Breakdown Spectroscopy (LIBS) /
- principle /
- physical mechanism

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图 1 共线型和正交型以及交叉型双脉冲激光配置图^{[

32
]}(激光1先入射激光2后入射)(改编自文献[ 32 ])

Figure 1. Collinear, orthogonal and crossed dual-pulse laser configurations^{[
32
]} (laser 2 is incident after laser 1) (adapted from Ref. [ 32 ])

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图 2 各种二级过程的时间尺度^{[
31
]} (改编自文献[ 31 ])

Figure 2. Time scale of the various secondary processes^{[
31
]}. (adapted from Ref. [ 31 ])

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图 3 等离子体冲击波前沿位置(R)随时间变化的Log(R)-log(T)图^{[
71
]}

Figure 3. Log(R)-log(T) plot of plasma shock front position (R) as a function of time^{[
71
]}. Reprinted with permission from Ref.[ 71 ]©Journal of Laser Applications.

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图 4 在激光能量为50 mJ、70 mJ和95 mJ时，VO的等离子体温度(T _e)与采集延时(t _d)的函数关系^{[
72
]}

Figure 4. The plasma temperature (T _e) of VO as a function of acquisition time delay (t _d) at laser energies of 50 mJ, 70 mJ, and 95 mJ ^{[
72
]}. Reprinted with permission from Ref.[ 72 ]© Journal of Atomic and Molecular Physics.

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图 5 在激光能量为50 mJ、70 mJ和95 mJ时，V₂O₃的电子密度(N _e)与采集延时(t _d)的函数关系^{[
72
]}

Figure 5. The electron density (N _e) of V₂O₃ as a function of acquisition time delay (t _d) at laser energies of 50 mJ, 70 mJ, and 95 mJ^{[
72
]}. Reprinted with permission from Ref.[ 72 ]©Journal of Atomic and Molecular Physics.

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表 1 LIBS定量分析性能的物理机制影响因素及受影响特性

Table 1. Factors influencing the physical mechanism of LIBS quantitative analysis performance and affected properties

影响因素	受影响特性
双脉冲	①等离子体的寿命，第一束激光剥蚀出的颗粒不仅被第一束激光产生的等离子体激发，还被第二束激光产生的等离子体再次激发，等离子体寿命被延长；②电子温度，第一束激光产生的等离子体对样品进行加热，使得第二束激光剥蚀量增加，电子温度升高；③样品表面气体环境密度，第一束激光产生的高温和等离子体的膨胀使样品表面产生一个大气密度较低的区域，第二束激光在此区域内对剥蚀颗粒进行激发可以获得更好的信号强度
脉冲宽度	①在相同的延迟时间下，等离子温度会随激光脉冲宽度的增加而升高；②在相同的延迟时间下ns脉冲激光的谱线强度比fs脉冲激光的谱线强度更高；③对于fs激光脉冲，烧蚀过程是直接从固体向蒸汽(或固向等离子体)转变，不存在热传导过程；对于ps激光脉冲，激光烧蚀伴随着电子热传导和目标内熔融区的形成；对于ns激光脉冲,会产生相对较大的熔融材料层
激光能量	①在同一延迟时间下，激光能量越高等离子体温度和电子数密度越大；②随着激光能量的增加，吸收呈指数增长，在高能量下达到饱和；③在较高能量时，烧蚀质量增加，等离子体内部具有更高的能量而呈半球状向外膨胀；而能量较低时，烧蚀质量较小，等离子体趋向于盘状
环境气体	①环境气体对等离子体的屏蔽效应影响很大，相比于空气环境氩气产生较高的等离子体温度,高的电子密度,消融速率较低,被探测元素的辐射强度较高；②在低的环境压力下,消融蒸汽可以自由的扩散,等离子体外部比内部的温度低,因为外部损失的能量较大。当提高压力时,由于环境气体限制了能量损失,使能量扩散更均一
靶材性质	①在只考虑金属样品时，基体效应对等离子体参数的影响很弱；②样品的物理性质和结构以及组分都会对等离子体产生影响，并且烧蚀质量与靶材硬度成反比。③靶材温度也会影响光谱强度和等离子体性质，谱强度随着温度的升高而增强
等离子体寿命	①等离子体寿命的变化会影响光谱信号的宽度和强度。当等离子体寿命较短时，产生的光谱信号较窄且信号强度较弱，而当等离子体寿命较长时，产生的光谱信号将更宽且信号强度更大
延时时间和积分时间	①当延时时间较短时，等离子体没有充分形成，所得到的光谱信号较小；而当延时时间过长时，等离子体可能因为散射或扩散而消失，同样会降低光谱信号的强度。②较短的积分时间可能会导致噪声的增加，而较长的积分时间则会提高信号质量，提高光谱信号的信噪比，但会降低测量速度

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