射频高气压混合气体放电数值研究
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摘要
高气压射频放电是产生等离子体的一种普遍的技术手段,长期以来被广泛的应用在材料表面改性、刻蚀和薄膜沉积等技术领域中。由于氩气、氮气和氧气成本低廉,因此常被用来作为气体放电的工作气体。相对于纯单一气体的高气压射频放电,高气压混合气体射频放电的产生机理和放电现象更为复杂。此外,在高气压混合气体放电中的各种放电参数,特别是气体压强、驱动频率、混合气体比例等对放电技术有着至关重要的影响,掌握这种影响可以提高高气压混合气体放电的工艺性能。为此,本文采用数值模拟的方法对混合气体高气压射频放电过程进行了研究。
本文工作主要分两部分来研究高气压下的混合气体放电现象。第一部分工作基于一维流体模型对采用诱导等离子体放电方法的高气压氮气射频放电进行了数值模拟研究,具体研究包括两个方面：(a)研究了高气压氮气注入时间和初始诱导氩等离子体的压强对高气压氮气射频放电特性的影响；(b)研究了驱动频率对带有诱导氩等离子体的高气压氮气射频放电的影响；第二部分的工作主要数值研究了大气压氮气和氧气混合气体射频放电现象,具体包括两个方面：(a)研究了不同混合比例气体对射频大气压氮气和氧气混合气体放电特性的影响。(b)研究了在固定氮氧混合比例下的大气压射频混合气体放电初期的等离子体特性。
本文共分六章,每章内容如下：
第一章为绪论,主要介绍高气压放电和混合气体放电的研究历史与现状。
第二章,基于一维流体模型利用有限差分法对相应的方程组进行离散,并且运用Fortran编程语言对模型进行编程计算,从而得到在200Torr气压下等离子体中的粒子密度、相应电子温度以及电场的空间分布。分别考虑了氮气的注入时间和初始诱导氩等离子体的压强对高气压氮气射频放电特性的影响。模拟结果显示,采用诱导氩等离子体放电方法可以在相对较低的条件下产生高气压放电等离子体。研究结果还表明,随着氮气注入时间的增加,等离子体密度先增加后趋于不变,电子温度先减少后趋于不变。随着初始诱导氩等离子体压强的增加,等离子体密度增加,电子温度下降。
第三章,基于一维流体模型继续研究了驱动频率对带有诱导氩等离子体的高气压氮气射频放电特性的影响。研究表明：当驱动频率从20MHz增加到100MHz时,电子密度、离子密度和中性粒子密度随着驱动频率的增加而增加。在此过程中,虽然电流密度发生了变化,但研究分析表明在整个过程中放电都处于稳定的α放电模式。随着驱动频率的增加,等离子体的电势、鞘层区域的电场强度和电子温度、等离子体区的长度增加,鞘层的厚度减小,等离子体区的电子温度有微小的下降。研究结果还表明在放电过程中,电子的产生率贯穿整个放电空间并且在鞘层区域出现峰值,这也进一步说明了放电是处于稳定的α模式放电。
第四章,由于氧气和氮气是空气的主要组成成分,因此研究大气压氮气和氧气的混合气体放电的特性对研究大气压空气放电有一定的帮助。本章利用一维流体模型,采用模拟方法研究了氧气所占比例对大气压氮氧混合气体射频放电的影响。研究结果表明随着氧气所占比例由4%增加到20%,电子和N4+离子的密度先减小后增加,O2+离子和。-离子密度增加,电子温度增加。当混合气体中氧气所占比例小于12%时,主要的负粒子是电子；当氧气所占比例大于12%时,主要的负粒子是O-离子。
第五章,基于一维流体模型,在这一章中对大气压氮氧混合气体放电做了进一步的研究,利用流体数值模拟的方法研究了包括13种反应粒子(例如：e,N2+,N4+,O2,O-, O+,NO+,N2(A1∑u+),N2(a1∑-u),O2(a1△g),O,N,NO)和73种反应过程的固定混合比例的大气压氮氧混合气体射频放电初期等离子体的特性。研究结果表明：在放电初期,负离子增加的速度要远大于其它的正离子增加的速度,电子增加的速度最慢,电子密度经历了先减小后缓慢增加的过程。在放电初期,主要的负粒子是O-离子,它比电子密度高3个数量级。研究结果还表明：电极间距对等离子体的特性有重要的影响,随着放电电极间距的增加,电子密度、N4+离子密度、O2+离子密度和O-离子密度增加。
最后,对全文进行总结并给出创新点和展望。
High pressure RF discharge is a main technology for producing plasma, it is also widely used to modify the surface properties of materials, etch and film deposition and other technology fields. Since argon, oxygen and nitrogen are cheap, they are usually used as working gas in discharge. Compared with the pure gas discharge, the mechanism and phenomena of mixture gases discharge at high pressure are more complicated. Besides, the parameters of high pressure RF discharge, particularly gas pressure, driven frequency and mixture ratio have important relationships with the discharge. To get these relationships can help to improve the plasma technology. This dissertation used a numerical simulation to study the mixture gases RF discharge at high pressure.
In this dissertation we have mainly studied for two aspects. First of all, based on a fluid model, induced plasma discharge approach has been adopted to numerically study nitrogen discharge at high pressure. It includes as the followings:(a) the effect of the time of adding nitrogen gas and initial induced argon plasma pressure on nitrogen discharge characteristics at high pressure has been studied;(b) the effect of RF frequency on nitrogen discharge with induced argon plasma in high pressure has also been studied; Secondly, in the dissertation we also have studied mixture gases atmospheric pressure RF discharge, including the effect of the concentration of O2in N2on nitrogen and oxygen atmosphere discharge and investigating the characteristics of nitrogen and oxygen RF atmospheric pressure discharge with fixed mixture gases ratio and the effect of gap distance on the plasma characteristics.
There are six chapters in this dissertation. The contents in each chapter are as follows:
Chapter1is the introduction. It introduces the history and present conditions of high pressure discharge and mixture gases discharge.
In chapter2, one-dimensional fluid model under drift/diffusion approximation was introduced. The model was solved by a finite difference model. A code by FORTRAN language has been developed to simulate the model. The electron density, ions densities, neutral particles densities, electron temperature and electric filed in spatial at200Torr are obtained. In this chapter we investigate the effect of the time of adding nitrogen gas and initial induced argon plasma pressure on discharge characteristics. The simulation results show that when the induced argon plasma exists, the nitrogen plasma in the relatively low conditions can be obtained. And during the process of the gas pressure increasing from1Torr to200Torr, the instability doesn't appear. Moreover the results also show that the slower rate of varying gas pressure, the plasma density is higher and the electron temperature is smaller; with the initial induced argon plasma pressure increasing, the charged particle densities increase, and electron temperature decreases.
In chapter3, based on one-dimensional plasma fluid model, the effect of the drive frequency on RF nitrogen discharge at high pressure with argon induced plasma has been further investigated. The numerical results show that through modulating the driven frequency, the discharge can obtain higher plasma density. Moreover, as the driven frequency increasing, the plasma voltage increases, the electric-field in sheath increases, the length of the plasma increases, the thickness of sheath decreases; the electron temperature in sheath increases obviously and has a small reduction in bulk plasma; the electron production rate is across the whole gap and has peak value in sheath. The discharge is in a mode.
In chapter4, the nitrogen gas and oxygen gas are the main components of air; therefore it is important to investigate the nitrogen and oxygen mixture gas discharge at atmospheric pressure. In this chapter, we studied the effect of the concentration of O2in N2on nitrogen and oxygen mixture gases atmosphere discharge. The numerical results show that when the concentration of O2in N2is less than12%, as the amount of O2grows, the electron density and N4+density decrease; the main negative particle is electron. And when the concentration of O2in N2is greater than12%, the electron density and N4+density increase with the increasing of oxygen; the main negative particle is O-. Moreover, O-density, O2density, electron temperature and the mixture gases electronegativity are increasing with the growth of O2in range of20%O2.
In chapter5, a one-dimensional fluid model is used for studying atmosphere discharge in mixture of nitrogen and oxygen. In the model, some particles, such as e, N2, N4+,O2+,O-, O+, NO+, N2(A1∑n+), N2(a+1∑-"), O2(a1△g),O, N, NO, are taken into account, as well as their73main reactions. The model is solved numerically and the evolutions of the spatial distributions of the particle densities are obtained. It shows that the density of negative ion increases more quickly than densities of positive ions and the densities of positive ions increase more quickly than electron density. The main charged particle is O-, whose density is much higher than other ions and electron. Discharge gap distance has effect on discharge properties. As the gap distance increasing the particles densities increase with it.
Finally, a brief summary ends this thesis.
本文工作主要分两部分来研究高气压下的混合气体放电现象。第一部分工作基于一维流体模型对采用诱导等离子体放电方法的高气压氮气射频放电进行了数值模拟研究,具体研究包括两个方面：(a)研究了高气压氮气注入时间和初始诱导氩等离子体的压强对高气压氮气射频放电特性的影响；(b)研究了驱动频率对带有诱导氩等离子体的高气压氮气射频放电的影响；第二部分的工作主要数值研究了大气压氮气和氧气混合气体射频放电现象,具体包括两个方面：(a)研究了不同混合比例气体对射频大气压氮气和氧气混合气体放电特性的影响。(b)研究了在固定氮氧混合比例下的大气压射频混合气体放电初期的等离子体特性。
本文共分六章,每章内容如下：
第一章为绪论,主要介绍高气压放电和混合气体放电的研究历史与现状。
第二章,基于一维流体模型利用有限差分法对相应的方程组进行离散,并且运用Fortran编程语言对模型进行编程计算,从而得到在200Torr气压下等离子体中的粒子密度、相应电子温度以及电场的空间分布。分别考虑了氮气的注入时间和初始诱导氩等离子体的压强对高气压氮气射频放电特性的影响。模拟结果显示,采用诱导氩等离子体放电方法可以在相对较低的条件下产生高气压放电等离子体。研究结果还表明,随着氮气注入时间的增加,等离子体密度先增加后趋于不变,电子温度先减少后趋于不变。随着初始诱导氩等离子体压强的增加,等离子体密度增加,电子温度下降。
第三章,基于一维流体模型继续研究了驱动频率对带有诱导氩等离子体的高气压氮气射频放电特性的影响。研究表明：当驱动频率从20MHz增加到100MHz时,电子密度、离子密度和中性粒子密度随着驱动频率的增加而增加。在此过程中,虽然电流密度发生了变化,但研究分析表明在整个过程中放电都处于稳定的α放电模式。随着驱动频率的增加,等离子体的电势、鞘层区域的电场强度和电子温度、等离子体区的长度增加,鞘层的厚度减小,等离子体区的电子温度有微小的下降。研究结果还表明在放电过程中,电子的产生率贯穿整个放电空间并且在鞘层区域出现峰值,这也进一步说明了放电是处于稳定的α模式放电。
第四章,由于氧气和氮气是空气的主要组成成分,因此研究大气压氮气和氧气的混合气体放电的特性对研究大气压空气放电有一定的帮助。本章利用一维流体模型,采用模拟方法研究了氧气所占比例对大气压氮氧混合气体射频放电的影响。研究结果表明随着氧气所占比例由4%增加到20%,电子和N4+离子的密度先减小后增加,O2+离子和。-离子密度增加,电子温度增加。当混合气体中氧气所占比例小于12%时,主要的负粒子是电子；当氧气所占比例大于12%时,主要的负粒子是O-离子。
第五章,基于一维流体模型,在这一章中对大气压氮氧混合气体放电做了进一步的研究,利用流体数值模拟的方法研究了包括13种反应粒子(例如：e,N2+,N4+,O2,O-, O+,NO+,N2(A1∑u+),N2(a1∑-u),O2(a1△g),O,N,NO)和73种反应过程的固定混合比例的大气压氮氧混合气体射频放电初期等离子体的特性。研究结果表明：在放电初期,负离子增加的速度要远大于其它的正离子增加的速度,电子增加的速度最慢,电子密度经历了先减小后缓慢增加的过程。在放电初期,主要的负粒子是O-离子,它比电子密度高3个数量级。研究结果还表明：电极间距对等离子体的特性有重要的影响,随着放电电极间距的增加,电子密度、N4+离子密度、O2+离子密度和O-离子密度增加。
最后,对全文进行总结并给出创新点和展望。
High pressure RF discharge is a main technology for producing plasma, it is also widely used to modify the surface properties of materials, etch and film deposition and other technology fields. Since argon, oxygen and nitrogen are cheap, they are usually used as working gas in discharge. Compared with the pure gas discharge, the mechanism and phenomena of mixture gases discharge at high pressure are more complicated. Besides, the parameters of high pressure RF discharge, particularly gas pressure, driven frequency and mixture ratio have important relationships with the discharge. To get these relationships can help to improve the plasma technology. This dissertation used a numerical simulation to study the mixture gases RF discharge at high pressure.
In this dissertation we have mainly studied for two aspects. First of all, based on a fluid model, induced plasma discharge approach has been adopted to numerically study nitrogen discharge at high pressure. It includes as the followings:(a) the effect of the time of adding nitrogen gas and initial induced argon plasma pressure on nitrogen discharge characteristics at high pressure has been studied;(b) the effect of RF frequency on nitrogen discharge with induced argon plasma in high pressure has also been studied; Secondly, in the dissertation we also have studied mixture gases atmospheric pressure RF discharge, including the effect of the concentration of O2in N2on nitrogen and oxygen atmosphere discharge and investigating the characteristics of nitrogen and oxygen RF atmospheric pressure discharge with fixed mixture gases ratio and the effect of gap distance on the plasma characteristics.
There are six chapters in this dissertation. The contents in each chapter are as follows:
Chapter1is the introduction. It introduces the history and present conditions of high pressure discharge and mixture gases discharge.
In chapter2, one-dimensional fluid model under drift/diffusion approximation was introduced. The model was solved by a finite difference model. A code by FORTRAN language has been developed to simulate the model. The electron density, ions densities, neutral particles densities, electron temperature and electric filed in spatial at200Torr are obtained. In this chapter we investigate the effect of the time of adding nitrogen gas and initial induced argon plasma pressure on discharge characteristics. The simulation results show that when the induced argon plasma exists, the nitrogen plasma in the relatively low conditions can be obtained. And during the process of the gas pressure increasing from1Torr to200Torr, the instability doesn't appear. Moreover the results also show that the slower rate of varying gas pressure, the plasma density is higher and the electron temperature is smaller; with the initial induced argon plasma pressure increasing, the charged particle densities increase, and electron temperature decreases.
In chapter3, based on one-dimensional plasma fluid model, the effect of the drive frequency on RF nitrogen discharge at high pressure with argon induced plasma has been further investigated. The numerical results show that through modulating the driven frequency, the discharge can obtain higher plasma density. Moreover, as the driven frequency increasing, the plasma voltage increases, the electric-field in sheath increases, the length of the plasma increases, the thickness of sheath decreases; the electron temperature in sheath increases obviously and has a small reduction in bulk plasma; the electron production rate is across the whole gap and has peak value in sheath. The discharge is in a mode.
In chapter4, the nitrogen gas and oxygen gas are the main components of air; therefore it is important to investigate the nitrogen and oxygen mixture gas discharge at atmospheric pressure. In this chapter, we studied the effect of the concentration of O2in N2on nitrogen and oxygen mixture gases atmosphere discharge. The numerical results show that when the concentration of O2in N2is less than12%, as the amount of O2grows, the electron density and N4+density decrease; the main negative particle is electron. And when the concentration of O2in N2is greater than12%, the electron density and N4+density increase with the increasing of oxygen; the main negative particle is O-. Moreover, O-density, O2density, electron temperature and the mixture gases electronegativity are increasing with the growth of O2in range of20%O2.
In chapter5, a one-dimensional fluid model is used for studying atmosphere discharge in mixture of nitrogen and oxygen. In the model, some particles, such as e, N2, N4+,O2+,O-, O+, NO+, N2(A1∑n+), N2(a+1∑-"), O2(a1△g),O, N, NO, are taken into account, as well as their73main reactions. The model is solved numerically and the evolutions of the spatial distributions of the particle densities are obtained. It shows that the density of negative ion increases more quickly than densities of positive ions and the densities of positive ions increase more quickly than electron density. The main charged particle is O-, whose density is much higher than other ions and electron. Discharge gap distance has effect on discharge properties. As the gap distance increasing the particles densities increase with it.
Finally, a brief summary ends this thesis.
引文
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