Two-dimensional images of radiative and metastable excited stateradial profiles for an inductively coupled plasma in argon

Inductively coupled plasma (ICP) was shown to be characterized by a substantial degree of stepwise excitation due to a large density of metastable atoms and an even larger population of electrons. The kinetics of metastables strongly affects the structure of the discharge and we have applied laser absorption spectroscopy to establish the density profile of argon metastables Ar(1s₅) in a single turn coil geometry. At the same time the radial profiles of the radiative Ar(3p₅) state obtained by using a computer-aided tomography are significantly different indicating the effect of electron induced quenching and stepwise processes in kinetics of the two states     

Two-dimensional observation of excited atoms and ions and excitation temperature in inductively coupled plasma using newly developed four channel spectrovideo camera

Abstract  

A four-channel spectrovideo camera was developed and applied to the measurement of spatially and spectrally resolved profiles of atomic and ionic emission in an inductively coupled plasma (ICP). Spatial distributions of argon and chromium atoms and iron ions in ICP were visualized successfully. The excitation temperature profiles of argon, chromium, and iron in ICP were also successfully constructed on the basis of the two-line method. The excitation temperature profiles obtained with a monochromator and the spectrovideo camera were in fairly good agreement.     

大气压氩气/空气针-环式介质阻挡放电发射光谱诊断

为了更加深入地了解氩气/空气等离子体射流内的电子输运过程及化学反应过程,通过针-环式介质阻挡等离子体发生器在放电频率10 kHz,一个大气压条件下对氩气/空气混合气进行电离并产生了稳定的等离子体射流。通过发射光谱法对不同峰值电压下氩气/空气等离子体射流的活性粒子种类、电子激发温度及振动温度进行了诊断。结果表明,射流中的主要活性粒子为N₂的第二正带系、Ar Ⅰ原子以及少量的氧原子,其中N₂的第二正带系的相对光谱强度最强、最清晰,在本试验的发射光谱中没有发现N+₂的第一负带系谱线,这说明在氩气/空气等离子体射流中几乎没有电子能量高于18.76 eV的自由电子。利用Ar Ⅰ原子激发能差较大的5条谱线做最小二乘线性拟合对等离子体射流的电子激发温度进行了计算,得到大气压氩气/空气等离子体射流的电子激发温度在7 000~11 000 K之间。随峰值电压的增大,电子激发温度表现出先增大后减小的变化趋势,这说明电子激发温度并不总是随峰值电压的增长单调变化的。通过N₂的第二正带系对等离子体振动温度进行了诊断,发现大气压氩气/空气等离子体射流振动温度在3 000~4 500 K之间,其随峰值电压的增大而减小,这意味着虽然峰值电压的提高可有效提高自由电子的动能,但当电子动能较大时自由电子与氮分子之间的相互作用时间将会缩短,进而二者之间的碰撞能量转移截面将会减小,从而导致等离子体振动温度的降低。     

Comparative Study on Excitation Mechanism of Chromium Emission Lines in Argon Radio‐Frequency Inductively‐Coupled Plasma,Nitrogen Microwave Induced Plasma,and Argon or Nitrogen Glow Discharge Plasmas

Boltzmann plots of both atomic and ionic chromium emission lines are investigated to compare the excitation mechanisms in four different plasmas: an argon inductively‐coupled plasma (Ar‐ICP), a nitrogen high‐power microwave induced plasma (N₂‐MIP), an argon glow discharge plasma (Ar‐GDP), and a nitrogen glow discharge plasma (N₂‐GDP). The plots of the atomic lines and the ionic lines give both linear relationships as well as similar excitation temperatures in the case of the Ar‐ICP, the N₂‐MIP, and the N₂‐GDP. It implies that a thermodynamic process such as electron collision would control their excitations. However, only in the case of the ionic‐line plot in the Ar‐GDP, a departure from linear relationship is observed and the estimated excitation temperature is rather higher than that with the atomic lines, meaning that a specific excitation mechanism exists in the Ar‐GDP. A possible explanation for these results is that a charge‐transfer collision between chromium atom and argon ion plays a dominant role in exciting highly‐lying energy levels of chromium ion, especially in the Ar‐GDP.     

大气压下绝缘毛细管内等离子体放电及其特性研究

在石英毛细管内利用两个边缘锋利的中空针型电极间的放电形成了63 cm长的大气压弧光等离子体.通过记录放电图片和测量电流-电压特征波形及伏安特性曲线的方法对管内等离子体从反常辉光状态过渡至超长弧光状态的过程做了细致的研究,发现管内等离子体在弧光状态下的电子密度不低于10¹⁴ cm^-3.另外,还进一步考察了两电极的间距和电源工作频率对放电伏安特性的影响以及通过发射光谱法测得的等离子体气体温度随外加电压的变化规律.当活性气体(氧气)按一定比例混合到氩等离子体中时,通过 关键词： 大气压等离子体 反常辉光放电 弧光放电 发射光谱     

低压氩气电感耦合等离子体特性分析及光谱诊断

电感耦合等离子体具有电子密度高、放电面积大、工作气压宽、结构简单等特点,在等离子体隐身领域具有突出的潜在优势。相对于开放式等离子体,闭式等离子体更适应于飞行器表面空气流速高、气压变化大的特殊环境。研究着眼于飞行器关键部件的局部隐身应用,设计了一种镶嵌于不锈钢壁中的圆柱形石英腔体结构,利用电感耦合放电的方式在腔体中产生均匀的平板状等离子体。由于增加了接地金属,降低了腔体内的钳制电位,同之前的纯石英腔体相比,该结构显著改善了等离子体的均匀性。研究了该闭式腔体内氩气电感耦合等离子体（ICP）的放电特性和发射光谱,实验中放电功率达到150 W时,可以明显观察到ICP的E-H模式转换,此时发射光谱和电子密度都呈现阶跃式增长。氩气发射光谱强度随放电功率升高显著增加,但是不同谱线强度增加幅度并不一致,分析认为是受不同的跃迁概率和激发能的影响。根据等离子体的发射光谱,利用玻尔兹曼斜率法对电子激发温度进行诊断,得到电子激发温度在2 000 K以上,并且随功率升高而降低,因为功率增大使电子热运动增强,粒子间的碰撞加剧,碰撞导致的能量消耗也更大。电子激发温度沿腔体径向呈近似均匀分布,分布趋势受功率影响不大。针对利用发射光谱诊断电子密度误差较大、计算繁琐的问题,引入Voigt卷积函数,经过拟合滤除多余展宽项的影响,得到准确的Stark展宽半高宽。最终利用发射光谱Stark展宽法计算了电子密度,腔体中心处的峰值密度可以达到7.5×1017 m-3。随着放电功率增大,线圈中容性分量降低,耦合效率增大,电子密度随之增大,但空间分布趋势基本不受功率影响。     

Excitation of Doubly‐Charged Ion Emission Lines from a Grimm‐Style Glow Discharge Plasma—Comparison Between Yttrium and Zirconium

Spectra of yttrium and zirconium emitted from a Grimm‐style glow discharge plasma were investigated to elucidate the excitation mechanism of doubly‐charged ionic lines when using argon–helium mixed gas as well as argon gas alone. The energy sum for exciting doubly‐charged ion species of yttrium is slightly smaller compared to the case of zirconium, which yields an interesting correlation in the excitation energy between their ionic species and excited species of helium or argon. The Y III emission lines which were assigned to the 4p⁶5p–4p⁶5s(4p⁶4d) transitions could be observed in the argon–helium mixed gas plasma, but those were hardly excited with argon gas only. The Zr III emission lines did not appear in the spectra emitted by the argon gas plasma nor by the mixed gas plasma. A possible explanation for these phenomena is that the excitation of these ionic species is caused principally by collisional energy transfer from helium species to the analyte atoms.     

氩气压力对螺旋波放电影响的发射光谱诊断及仿真研究

螺旋波等离子体源以其高电离效率与高密度优势受到多个领域的青睐。螺旋波放电高电离效率的机理或者功率耦合模式,一直是困扰该领域学者的难点之一,对于放电过程与特性的诊断则是揭示其物理机制的重要途径。光谱诊断能够克服介入式诊断手段对等离子体的干扰同时受等离子体烧蚀等弊端,且响应速度快、操作灵活。为研究螺旋波等离子体的放电特性以及气体压力的影响,开展了以氩气为工质气体的光谱实验研究,并针对实验开展了Helic程序数值模拟。通过改变光纤探头焦距调整径向诊断位置,得到谱线强度的径向分布。由氩原子4p-4s能级跃迁产生的谱线主要集中在740～920 nm区间,谱线相对强度较离子激发谱线较强。实验研究发现,在较低氩气压力范围（0.2 Pa<P_Ar<1.0 Pa）,随着压力增加,放电光强迅速增加,但是当压力增加到大于1.0 Pa之后,光强增长的趋势变缓,甚至部分谱线的相对强度不再增长,达到类饱和状态,朗缪尔探针测量得到离子密度变化趋势与其相似。光强分布在靠近径向边界处（r≈4 cm）存在凸起,且随压力增加,该凸起分布更为明显。通过对电子温度的计算发现,压力增加到一定程度将影响放电均匀性。仿真结果显示,增大压力,功率沉积密度的径向分布逐渐向径向边界处积累,与实验观察到的谱线强度径向凸起相一致,螺旋波与TG波的耦合效率增加。随着气体压力的增加,E_r的径向边界峰值降低,原因是波所受阻尼增强,TG波被有效地局限于径向较窄的边界处。电流密度轴向分量J_z在等离子体内部和边界处的峰值呈显著的减小趋势,可见,虽然压力增加一定程度上提高了等离子体密度,但却相应的减小了电离率,导致轴向电流密度受限。但是径向电流密度J_r却呈现先减小后增大的趋势,且增长幅度明显,综合来看,放电效率有所提高。可见适当增加气体压力,有助于提高放电的功率耦合效率和强度,增加等离子体密度。光强比值法是针对线性谱线参数计算的典型方法,Helic程序亦是专业领域内认可度很高的计算工具,结果可靠,分析方法具有可借鉴性。实验及仿真结果对于提高氩气工质下的螺旋波放电强度提供了一定的参考价值。     

短管螺旋波放电中等离子体参数测量和模式转化研究

对长度为45 cm的短放电管螺旋波放电等离子体进行了Langmuir探针、原子发射光谱以及集成电荷耦合检测器(ICCD)检测诊断,研究螺旋波等离子体的放电特性.Langmuir探针数据显示电子密度在射频功率增加过程中出现两次大幅增长,由此确认了放电模式的转换及螺旋波放电模式的出现.发射光谱测量结果与Langmuir探针测量的电子密度数据一致,发现Ar原子和Ar离子的谱线强度与放电模式变化有着密切相关性.而通过对不同放电模式的ICCD测量,获得射频功率吸收因放电模式转变而变化的方式,认为放电模式转换时电子行为和能量传递方式也发生着变化.     

A spectroscopic investigation of stabilized dc argon arc at atmospheric pressure by power modulation technique

Spatial distribution of delayed responses of argon and hydrogen spectral line and continuum intensity to square power modulation was investigated in order to get better insight into the processes occurring in argon dc arc plasma. The power was abruptly changed between stationary values, 9 and 3.5 A. For these currents steady state radial distributions of electron number density, temperature and emission intensity were measured. On part of the discharge radial profiles the power drop and the power jump are both accompanied by intensity peaks which may be explained by displacement of the arc core axis and change in the arc core diameter during the power modulation.     

发射光谱研究氩气/空气混合气体介质阻挡放电能量传递过程

使用水电极介质阻挡放电装置,对比氩气与氩气/少量空气的混合气体以及空气与空气/少量氩气的混合气体放电的发射光谱,研究了氩气与空气相混合时气体放电中的能量传递过程。实验发现, 当氩气中加入少量的空气时,氩原子谱线均变弱,说明空气中的氮分子对氩原子的各激发态具有猝灭作用。并且随着空气含量的增加,各谱线变弱的速率不同。越是与氮分子的激发电位接近的氩原子的激发态被猝灭的作用越明显。另一方面,当空气中加入少量氩气时,发现氮分子第二正带系和氮分子离子第一负带系的谱线均被增强。说明在空气/少量氩气放电中,氮分子的激发由于亚稳态氩原子的潘宁激发传能而增强。因此在氩气/空气混合气体放电中,气体成分及比例影响放电的发光特性和能量传输特性。     

高通鸟笼线圈激发螺旋波等离子体特性研究

研制了高通鸟笼线圈,使用氩气作为工质气体对射频天线的工作性能进行了初步评估。利用COMSOL5.4模拟出了鸟笼天线在13.56MHz的工作频率下,电场和磁场呈线性极化分布。对鸟笼线圈进行了电路结构解剖,推导出了其谐振频率计算公式。利用热耦合红外测温仪测试了正常工作状态下的鸟笼线圈外表温度明显低于传统射频天线,电容器最高温度仅65.8°。使用光谱仪对螺旋波等离子体放电光谱特性进行诊断。通过朗缪尔探针诊断了不同压强和磁场强度下螺旋波等离子体密度,在1.0Pa、600Gs、射频功率700W条件下等离子体密度达到1.62×10¹⁸m^-3。诊断了正向功率和反向功率对应的等离子体密度,其与磁滞现象变化趋势雷同。测试了螺旋波等离子体的径向密度分布,其在轴心处密度达到最高。探究了无磁场条件下等离子体特性,其密度值不会发生大幅度跃迁,纵向磁场是引发螺旋波等离子体放电的关键因素,低压条件下有利于得到更低的电子温度,最低达到2.67eV。表明鸟笼线圈低热耗、高馈入的特性使其在激发大体积的高密度螺旋波等离子体方面具有明显优势,可以投入到下一阶段氢气螺旋波等离子体的激...     

Plasma Source Mass Spectrometric Analysis of Biological and Environmental Samples: Dealing with Potential Interferences

Introduction

Effectiveness of a plasma to dissociate the sample into ions has been the basis of the development of plasma source optical emission spectrometer (OES) and mass spectrometer (MS) for elemental and isotope analysis. Among the available ways of inducing and sustaining a plasma, only inductively coupled plasma (ICP) has gained commercial application. The ICP is an electrodeless discharge in a gas at atmospheric pressure, maintained by energy coupled to it from a radio frequency generator. This is done by a coupling coil, which functions as the primary of radio frequency transformer, the secondary of which is created by the discharge itself (Jarvis et al., 1992). An ICP-MS system consists of a plasma source (ICP) interfaced with a quadrupole MS. The plasma ionizes the elements of the sample and the MS serves as a detector that measures the mass to charge (m/z) ratio of the element(s) or isotope(s) of interest. Generally an argon (Ar) plasma is used, but other plasma sources have also been proposed (Brown et al., 1988; Satzger et al., 1987).     

Standing Waves along a Microwave Generated Surface Wave Plasma

Two surface wave plasma columns, generated by microwave power in argon at gas pressures of 0.05 torr to 330 torr, interact in the same discharge tube to form standing surface waves. Radial electric field Er and azimuthal magnetic field H? outside the discharge tube are measured to be 90° out of phase with respect to axial position and to decay exponentially with radial distance from the tube axis. Maximum light emission occurs at the position of maximum H?, and minimum Er. Electron temperature and density are measured at low pressures with double probes inserted into the plasma at a null of Er. Measured electron densities compare well with those predicted by Gould-Trivelpiece (GT) surface wave theory. Measured electron temperatures are the same order of magnitude as temperatures predicted by positive column theory.     

13.56 MHz/2 MHz柱状感性耦合等离子体参数的对比研究

通过Langmuir双探针和发射光谱诊断方法,对比研究了驱动频率为13.56 MHz和2 MHz柱状感性耦合等离子体中电子密度和电子温度的径向分布规律.结果表明:在高频和低频放电中,输入功率的增加对等离子体参数产生了不同的影响,高频放电中主要提升了电子密度,低频放电中则主要提升了电子温度.固定气压为10 Pa,分别由高频和低频驱动时,电子密度的径向分布均为"凸型".而电子温度的分布差异比较明显,高频驱动时,电子温度在腔室中心较为平坦,在边缘略有上升;低频驱动时,电子温度随径向距离的增加而逐渐下降.为了进一步分析造成这种差异的原因,在相同放电条件下采集了氩等离子体的发射光谱图,利用分支比法计算了亚稳态粒子的数密度,发现电子温度的径向分布始终与亚稳态粒子的径向分布相反.继续升高气压到100 Pa,发现不论高频还是低频放电,电子密度的径向分布均从"凸型"转变为"马鞍形",较低气压时电子密度的均匀性有了一定的提升,但低频的均匀性更好.     

Excited atoms in argon gas discharge plasma

General principles are discussed for a gas discharge plasma involving excited atoms where electron-atom collision processes dominate. It is shown that an optimal kinetic model of this plasma at not large electric field strengths can be based on the rate constants of quenching excited atom states by electron impact. The self-consistent character of atom excitation in gas discharge plasma is important and results in the tail of the energy distribution function of electrons being affected by the excitation process, which in turn influences the excitation rate. These principles are applied to an argon gas discharge plasma where excitation and ionization processes have a stepwise character and proceed via formation of argon atom states with the electron shell 3p ⁵4s.     

同轴空心阴极氦等离子体的电子激发温度研究

利用同轴空心阴极放电装置,产生氦低温等离子体。通过对等离子体的发射光谱进行测量和计算,研究放电功率以及氦气压强对等离子体的电子激发温度的影响。结果表明:氦低温等离子体的发射光谱主要由连续谱和原子谱线构成,放电功率和压强对谱线的强度具有明显影响。压强的变化不仅影响电子从电场中获得的能量,还会影响电子与原子的碰撞频率,从而导致电子激发温度随着氦气压强的增大,出现先上升后下降的变化趋势。     

A Linear Model for the Interpretation of Optical Emission Spectroscopy Measurements in Low Pressure DC Magnetron Sputtering

For a balanced dc magnetron discharge a linear model for the formation of excited and ionized species is presented. The consideration is based on collisional kinetic theory and a correlation of discharge current with ionization rates, and leads to normalized rate coefficients. The electron energy distribution changes according to the determining external parameters, but needs neither to be known in detail nor to be of Maxwellian type. The model calculations are consistent with measurements done by optical emission spectroscopy (OES) on the magnetron sputtering of aluminium in argon discharges. The dependences of optical emission intensities on discharge current and on argon pressure show that both, excited argon atoms as well as excited argon ions, are generated from neutral argon by direct, fast electron impact. It is additionally shown that at least for low argon pressure the excitation of aluminium atoms is also caused by direct electron impact.     

感应耦合等离子体的1维流体力学模拟

 采用双极扩散近似的流体力学模型，通过数值模拟方法研究了射频感应耦合等离子体(ICP)中等离子体密度和电子温度等物理量的空间分布，其中射频源的功率沉积由动力学理论给出。分析了不同的射频线圈的驱动电流和放电气压对等离子体密度和电子温度空间分布的影响。在低气压下，等离子体密度基本上保持空间均匀分布。随着放电压强的增加，等离子体密度的分布呈现出明显的空间不均匀性。当线圈电流增大时，等离子体密度和电子温度都随着增大。     

基于平面螺旋电感的微型ICP激发源

随着微电子机械系统(MEMS)技术的发展,基于MEMS的光谱仪分光系统和光电检测系统研究报道日益增多,但是微型激发源的研究报道相对较少。文章介绍了一种基于表面微机械加工技术的微型电感耦合等离子体(ICP)激发源,其RF功耗在数瓦以下、氩气消耗量远低于常规ICP激发源。阐述了这种激发源的结构、加工工艺流程及性能指标。同时还介绍了作者设计制作的基于PCB工艺的微型ICP激发源,采用了平面螺旋电感线圈和平面梳状交指电容,在100 Pa氩气气压下用13.56 MHz,3.5 W射频功率激励点燃了等离子体火炬,给出了装置的外观微型ICP火炬的照片。最后展望了该微型的ICP激发源在光谱仪中的应用前景。