等离子体基低能离子注入内表面鞘层特性的数值研究
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摘要
本文针对等离子体基低能离子注入(Plasma-Based Low-Energy Ion Implantation-PBLEII)技术改性金属圆管内表面,提出并建立了基于电子回旋共振(Electron Cyclotron Resonance-ECR)微波等离子体的PBLEII圆管内表面改性系统；利用磁化鞘层碰撞流体模型,模拟计算了磁场作用下离子注入能量、入射角度、注入剂量及鞘层扩展特性；研究了处理圆管临界半径与等离子体密度、脉冲负偏压、等离子体源半径及工作气压的关系,实现了PBLEII圆管内表面的工艺参数优化；利用发展的低压非稳态扩散流体模型,模拟计算了低脉冲负偏压和等离子体双极性扩散共同作用下,PBLEII圆管内表面脉冲鞘层演化规律及脉冲间隔内等离子体回复特性。旨在通过PBLEII内表面鞘层特性的数值研究,为制订PBLEII复杂表面改性的技术要求和工艺规范提供理论依据和指导。
研发的PBLEII圆管内表面改性装置,主要包括：真空室、线性ECR微波等离子体源、低能离子注入电源、辅助加热源等。线性ECR微波等离子体源由微波源、同轴线波导、接地栅网电极和真空室外磁场线圈构成。在同轴波导外导体上沿螺旋线均匀分布方式开设缝隙辐射窗口,同轴线和栅网电极之间获得由2.45GHz微波源产生的均匀能量微波,在直流线圈产生的0.0875T磁场作用下,产生轴向和周向均匀分布的、密度为101-～1011cm-3的ECR微波等离子体,低能离子注入电源向管壁施加-0.4--2kV的脉冲负偏压,加速管内壁鞘层内的离子,实现低能离子注入。利用离子连续性方程、包含磁场作用的运动方程、Poisson方程和电子Boltzmann关系的磁化鞘层碰撞流体模型,计算了圆管内表面低能离子注入过程中磁场对注入参数的作用和注入参数的轴向均匀性。在等离子体密度1010cm-3、脉冲负偏压-2kV、等离子体源半径2.0cm、工作气压10-2Pa下改性内径6.0cm圆管内表面,0.0875T轴向匀强磁场仅使圆管内部离子注入角度增大0-6°,对内表面改性效果影响较小,在PBLEII圆管内表面鞘层扩展数值计算中可忽略装置外加磁场作用；在远离管端的内表面上离子注入角度小于10°,注入能量在1600eV左右,而在圆管端向管内轴向约2.0cm区域内离子以较大角度10～60°和较低能量400～1600eV注入,离子注入剂量在远离管端处较均匀,注入剂量达到门槛值1017cm-2所需时间约为5.0h,在距管端0.5cm处注入剂量出现峰值,注入剂量达到门槛值10"cm-2所需时间约为3.1h。低能离子注入和热扩散相复合的传质过程中,离子注入剂量决定了改性效果,处理圆管管端附近改性效果较为均匀。
利用鞘层碰撞流体模型,计算了PBLEII所能处理的圆管半径与工艺参数的关系,在等离子体密度1010cm-3、脉冲负偏压-0.4--2kV、等离子体源半径1.0～2.0cm、工作气压10-2-10-1Pa下,改性时间10h里可保证内径10.0cm以下圆管获得1017cm-2的门槛值,-0.4--2kV的低脉冲负偏压可实现内径1.0cm圆管的有效注入；脉冲负偏压、等离子体源半径及工作气压是影响处理圆管上限尺寸的主要因素,等离子体密度1010cm-3、脉冲负偏压-2kV、等离子体源半径2.0cm,工作气压10-2Pa下,所能处理圆管内径上限值为26.5cm；脉冲负偏压稳定值和等离子体源半径是影响处理圆管下限尺寸的主要因素,脉冲负偏压-2kV,等离子体源半径0.93cm下,所能处理圆管内径下限值可达1.00cm。采用1010～1011cm-3的较高密度等离子体和-0.4～-2kV的低脉冲负偏压,PBLEII改性小尺寸圆管内表面可得到优异的改性效果。
基于等离子体在较低气压下的双极性扩散机制,假设等离子体在非稳态扩散过程中每一时刻都是准平衡态、准电中性,用Lieberman提出的低压稳态离子迁移率描述离子的瞬时通量,结合描述连续离子流的流体运动方程和电子Boltzmann关系,发展出普适性的低压非稳态扩散流体模型,计算了圆管内表面低能离子注入过程中等离子体扩散对鞘层扩展的作用、等离子体回复规律以及占空比对离子注入剂量的影响,在等离子体密度1010cm-3、电子温度8eV、脉冲负偏压-2kV、脉宽10μs、等离子体源半径2.0cm、工作气压10-1Pa下改性内径6.0cm圆管内表面,等离子体非稳态扩散能促进鞘层扩展,使鞘层尺度在脉冲结束时由1.96cm增大约0.31cm；高电子温度和低工作气压使等离子体的回复过程加快,脉冲结束后仅1.3μs即回复至稳态的95%,且在2.8μs出现了过冲现象,10.0μs以后趋于稳态；离子注入能量受占空比影响很小,高于0.8的占空比导致等离子体不完全回复,但高占空比能大幅提高离子注入效率。占空比为0.3时,平均注入离子流密度仅0.86×104A/cm2,而占空比为0.9时,平均注入离子流密度可达2.60×10-4A/cm2。0.9占空比可使管内壁在10h改性时间里获得5.8×1019cm-2的超高离子注入剂量,提高脉冲负偏压占空比是增加PBLEII圆管内表面改性离子注入剂量的有效途径。
For inner surface modification of metallic tube by plasma-based low-energy ion implantation (PBLEII), a PBLEII inner surface modification system which based on the electron cyclotron resonance microwave plasma is developed in this paper. Using magnetized sheath collisional fluid model, the ion implantation energy, angle, dose, and sheath evolution characteristics under additional magnetic field were studied. The dependence of critical radius of tube on plasma density, negative voltage bias, plasma source radius and processing pressure were studied and the optimization of the process parameters for the inner surface modification by PBLEII is realized. Using the developed low-pressure non-steady diffusion fluid model, the pulsed sheath dynamics and plasma recovery characteristics during pulse-off time of PBLEII inner surface modification under low negative voltage pulses and plasma bipolar diffusion were studied. The numerical study on sheath characteristics of plasma-based low-energy ion implantation for inner surface modification is made, in order to provide the theoretical basis and guidance for setting the technical requirement and process specification of complex surface modification by PBLEII.
The developed PBLEII device for inner surface modification of the tube includes vacuum chamber, linear ECR microwave plasma source, low-energy ion implantation power, auxiliary heating source, etc.. The linear ECR microwave plasma source is consist of microwave source, coaxial line waveguide, grounded grid electrode and magnetic field coil outside the vacuum chamber. Radiation slots were slotted along the spiral line on the outer conductor of the waveguide, and the2.45GHz microwave was obtained between the coaxial line and the grid electrode by microwave source along the slots. Under the effect of0.0875T magnetic field produced by magnetic field coil, the plasma of1010～1011ions cm-3density can be generated uniformly along the axial and tangential directions, low-energy ion implantation power applied-0.4～-2kV negative voltage pulses onto the tube, ions in the sheath of the inner surface were accelerated by the pulses and realized the low-energy ion implantation. Using equation of ion continuity, equation of ion motion which is consist of magnetic field, Poisson's equation and Boltzmann relation of electron, the magnetized sheath collisional fluid model is established, the effect of magnetic field on the parameters of low-energy ion implantation and the uniformity of implantation parameters along axial direction were studied, calculating plasma density1010ions cm-3, negative voltage pulses steady value-2kV, plasma source radius2.0cm, processing pressure10-2Pa, low-energy ion implanting the inner surface of the tube with6.0cm radius, the axial uniform magnetic field of0.0875T only increased the ion implantation angle inside the tube for0～6°, and had no disadvantageous effect on the inner surface modification process, the effect of magnetic field can be ignored. On the inner surface where far away from the ends of the tube, the ion implantation angle is less than10°, the ion implantation energy is about1600eV, but in the area where less than2.0cm from the ends of the tube, the ion implanted with a larger angle of10～60°and a smaller energy of400-1600eV. The ion implantation dose is uniform far away from the ends of the tube, the necessary time to achieve the implantation dose threshold1017ions cm-2is about5.0h, a implantation dose peak appeared at the position0.5cm away from the ends of the tube, and the necessary time to achieve the implantation dose threshold1017ions cm-2is about3.1h. In the mass transfer process which combined by low-energy ion implantation and thermal diffusion, the modification effect was determined by the ion implantation dose and therefore, an acceptable modification effect can be obtained onto the area at the ends of the tube due to the sufficient ion implantation dose.
Using the sheath collisional fluid model, the relationship of the radius of tube which can be treated by PBLEII and the processing parameters were studied, calculating plasma density1010ions cm-3, negative voltage pulses steady value-0.4～-2kV, plasma source radius1.0-2.0cm, processing pressure10-2～10-1Pa, modification time10h can provide1017ions cm-2implantation dose threshold for the radius of less than10.0cm tube, low negative voltage pulses of-0.4～-2kV can realize effective implantation of radius1.0cm tube theoretically; negative voltage pulses steady value, plasma source radius and processing pressure are the main influencing factors of the maximum radius of the tube, plasma density1010ions cm-3negative voltage pulses steady value-2kV, plasma source radius2.0cm, processing pressure10-2Pa, the maximum radius of tube is26.5cm; negative voltage pulses steady value and plasma source radius are the main influencing factors of the minimum radius of the tube, negative voltage pulses steady value-2kV, plasma source radius0.93cm, the minimum radius of the tube is1.00cm. For the high plasma density of1010～1011ions cm-3and low negative voltage pulses of-0.4～-2kV is used in the PBLEII process for inner surface modification, an acceptable effect can be obtained for small size tubes.
Based on the plasma ambipolar diffusion mechanism under relatively lower pressure, assuming that during the plasma non-steady diffusion process the plasma is quasi-equilibrium and quasi-neutrality in every moment, the ion instant flux is described by the low-pressure steady ion mobility proposed by Lieberman,combined with the fluid motion equation which described the continuous ion flux and Boltzmann relation of electron,the low-pressure non-steady diffusion fluid model is established, the effect of plasma diffusion on the sheath expansion, plasma recovery behavior and the effect of duty cycle on the ion implantation dose were studied. Calculating plasma density1010ions cm-3, electron temperature8eV, negative voltage pulses steady value-2kV, pulse width10μs, plasma source radius2.0cm, processing pressure10-1Pa, low-energy ion implanting the inner surface of tube with6.0cm radius, the non-steady diffusion of plasma can promote the sheath expansion, and the sheath size increased about0.31cm from1.96cm at the end of the pulse; high electron temperature and low processing pressure accelerate the plasma recovery process, which recovers to95%of the steady state just1.3μs after the end of the pulse, at2.8μs there is an overshoot phenomenon and after10.0μs the recovery gradually tends to steady state; the effect of duty cycle on the ion implantation energy is little, the duty cycle higher than0.8results in the plasma incomplete recovery, but high duty cycle can increase the ion implantation efficiency substantially. When the duty cycle is0.3, the average implanted ion current density is only0.86×10-4A/cm2, but when the duty cycle is0.9, the average implanted ion current density is up to2.60×10-4A/cm2. The duty cycle of0.9can provide the inner surface of the tube an ultrahigh ion implantation dose of5.8×1019ions cm-2during10h modification time. For the inner surface modification process by PBLEII, increasing the duty cycle of negative voltage pulses is an effective approach to increase the ion implantation dose.
研发的PBLEII圆管内表面改性装置,主要包括：真空室、线性ECR微波等离子体源、低能离子注入电源、辅助加热源等。线性ECR微波等离子体源由微波源、同轴线波导、接地栅网电极和真空室外磁场线圈构成。在同轴波导外导体上沿螺旋线均匀分布方式开设缝隙辐射窗口,同轴线和栅网电极之间获得由2.45GHz微波源产生的均匀能量微波,在直流线圈产生的0.0875T磁场作用下,产生轴向和周向均匀分布的、密度为101-～1011cm-3的ECR微波等离子体,低能离子注入电源向管壁施加-0.4--2kV的脉冲负偏压,加速管内壁鞘层内的离子,实现低能离子注入。利用离子连续性方程、包含磁场作用的运动方程、Poisson方程和电子Boltzmann关系的磁化鞘层碰撞流体模型,计算了圆管内表面低能离子注入过程中磁场对注入参数的作用和注入参数的轴向均匀性。在等离子体密度1010cm-3、脉冲负偏压-2kV、等离子体源半径2.0cm、工作气压10-2Pa下改性内径6.0cm圆管内表面,0.0875T轴向匀强磁场仅使圆管内部离子注入角度增大0-6°,对内表面改性效果影响较小,在PBLEII圆管内表面鞘层扩展数值计算中可忽略装置外加磁场作用；在远离管端的内表面上离子注入角度小于10°,注入能量在1600eV左右,而在圆管端向管内轴向约2.0cm区域内离子以较大角度10～60°和较低能量400～1600eV注入,离子注入剂量在远离管端处较均匀,注入剂量达到门槛值1017cm-2所需时间约为5.0h,在距管端0.5cm处注入剂量出现峰值,注入剂量达到门槛值10"cm-2所需时间约为3.1h。低能离子注入和热扩散相复合的传质过程中,离子注入剂量决定了改性效果,处理圆管管端附近改性效果较为均匀。
利用鞘层碰撞流体模型,计算了PBLEII所能处理的圆管半径与工艺参数的关系,在等离子体密度1010cm-3、脉冲负偏压-0.4--2kV、等离子体源半径1.0～2.0cm、工作气压10-2-10-1Pa下,改性时间10h里可保证内径10.0cm以下圆管获得1017cm-2的门槛值,-0.4--2kV的低脉冲负偏压可实现内径1.0cm圆管的有效注入；脉冲负偏压、等离子体源半径及工作气压是影响处理圆管上限尺寸的主要因素,等离子体密度1010cm-3、脉冲负偏压-2kV、等离子体源半径2.0cm,工作气压10-2Pa下,所能处理圆管内径上限值为26.5cm；脉冲负偏压稳定值和等离子体源半径是影响处理圆管下限尺寸的主要因素,脉冲负偏压-2kV,等离子体源半径0.93cm下,所能处理圆管内径下限值可达1.00cm。采用1010～1011cm-3的较高密度等离子体和-0.4～-2kV的低脉冲负偏压,PBLEII改性小尺寸圆管内表面可得到优异的改性效果。
基于等离子体在较低气压下的双极性扩散机制,假设等离子体在非稳态扩散过程中每一时刻都是准平衡态、准电中性,用Lieberman提出的低压稳态离子迁移率描述离子的瞬时通量,结合描述连续离子流的流体运动方程和电子Boltzmann关系,发展出普适性的低压非稳态扩散流体模型,计算了圆管内表面低能离子注入过程中等离子体扩散对鞘层扩展的作用、等离子体回复规律以及占空比对离子注入剂量的影响,在等离子体密度1010cm-3、电子温度8eV、脉冲负偏压-2kV、脉宽10μs、等离子体源半径2.0cm、工作气压10-1Pa下改性内径6.0cm圆管内表面,等离子体非稳态扩散能促进鞘层扩展,使鞘层尺度在脉冲结束时由1.96cm增大约0.31cm；高电子温度和低工作气压使等离子体的回复过程加快,脉冲结束后仅1.3μs即回复至稳态的95%,且在2.8μs出现了过冲现象,10.0μs以后趋于稳态；离子注入能量受占空比影响很小,高于0.8的占空比导致等离子体不完全回复,但高占空比能大幅提高离子注入效率。占空比为0.3时,平均注入离子流密度仅0.86×104A/cm2,而占空比为0.9时,平均注入离子流密度可达2.60×10-4A/cm2。0.9占空比可使管内壁在10h改性时间里获得5.8×1019cm-2的超高离子注入剂量,提高脉冲负偏压占空比是增加PBLEII圆管内表面改性离子注入剂量的有效途径。
For inner surface modification of metallic tube by plasma-based low-energy ion implantation (PBLEII), a PBLEII inner surface modification system which based on the electron cyclotron resonance microwave plasma is developed in this paper. Using magnetized sheath collisional fluid model, the ion implantation energy, angle, dose, and sheath evolution characteristics under additional magnetic field were studied. The dependence of critical radius of tube on plasma density, negative voltage bias, plasma source radius and processing pressure were studied and the optimization of the process parameters for the inner surface modification by PBLEII is realized. Using the developed low-pressure non-steady diffusion fluid model, the pulsed sheath dynamics and plasma recovery characteristics during pulse-off time of PBLEII inner surface modification under low negative voltage pulses and plasma bipolar diffusion were studied. The numerical study on sheath characteristics of plasma-based low-energy ion implantation for inner surface modification is made, in order to provide the theoretical basis and guidance for setting the technical requirement and process specification of complex surface modification by PBLEII.
The developed PBLEII device for inner surface modification of the tube includes vacuum chamber, linear ECR microwave plasma source, low-energy ion implantation power, auxiliary heating source, etc.. The linear ECR microwave plasma source is consist of microwave source, coaxial line waveguide, grounded grid electrode and magnetic field coil outside the vacuum chamber. Radiation slots were slotted along the spiral line on the outer conductor of the waveguide, and the2.45GHz microwave was obtained between the coaxial line and the grid electrode by microwave source along the slots. Under the effect of0.0875T magnetic field produced by magnetic field coil, the plasma of1010～1011ions cm-3density can be generated uniformly along the axial and tangential directions, low-energy ion implantation power applied-0.4～-2kV negative voltage pulses onto the tube, ions in the sheath of the inner surface were accelerated by the pulses and realized the low-energy ion implantation. Using equation of ion continuity, equation of ion motion which is consist of magnetic field, Poisson's equation and Boltzmann relation of electron, the magnetized sheath collisional fluid model is established, the effect of magnetic field on the parameters of low-energy ion implantation and the uniformity of implantation parameters along axial direction were studied, calculating plasma density1010ions cm-3, negative voltage pulses steady value-2kV, plasma source radius2.0cm, processing pressure10-2Pa, low-energy ion implanting the inner surface of the tube with6.0cm radius, the axial uniform magnetic field of0.0875T only increased the ion implantation angle inside the tube for0～6°, and had no disadvantageous effect on the inner surface modification process, the effect of magnetic field can be ignored. On the inner surface where far away from the ends of the tube, the ion implantation angle is less than10°, the ion implantation energy is about1600eV, but in the area where less than2.0cm from the ends of the tube, the ion implanted with a larger angle of10～60°and a smaller energy of400-1600eV. The ion implantation dose is uniform far away from the ends of the tube, the necessary time to achieve the implantation dose threshold1017ions cm-2is about5.0h, a implantation dose peak appeared at the position0.5cm away from the ends of the tube, and the necessary time to achieve the implantation dose threshold1017ions cm-2is about3.1h. In the mass transfer process which combined by low-energy ion implantation and thermal diffusion, the modification effect was determined by the ion implantation dose and therefore, an acceptable modification effect can be obtained onto the area at the ends of the tube due to the sufficient ion implantation dose.
Using the sheath collisional fluid model, the relationship of the radius of tube which can be treated by PBLEII and the processing parameters were studied, calculating plasma density1010ions cm-3, negative voltage pulses steady value-0.4～-2kV, plasma source radius1.0-2.0cm, processing pressure10-2～10-1Pa, modification time10h can provide1017ions cm-2implantation dose threshold for the radius of less than10.0cm tube, low negative voltage pulses of-0.4～-2kV can realize effective implantation of radius1.0cm tube theoretically; negative voltage pulses steady value, plasma source radius and processing pressure are the main influencing factors of the maximum radius of the tube, plasma density1010ions cm-3negative voltage pulses steady value-2kV, plasma source radius2.0cm, processing pressure10-2Pa, the maximum radius of tube is26.5cm; negative voltage pulses steady value and plasma source radius are the main influencing factors of the minimum radius of the tube, negative voltage pulses steady value-2kV, plasma source radius0.93cm, the minimum radius of the tube is1.00cm. For the high plasma density of1010～1011ions cm-3and low negative voltage pulses of-0.4～-2kV is used in the PBLEII process for inner surface modification, an acceptable effect can be obtained for small size tubes.
Based on the plasma ambipolar diffusion mechanism under relatively lower pressure, assuming that during the plasma non-steady diffusion process the plasma is quasi-equilibrium and quasi-neutrality in every moment, the ion instant flux is described by the low-pressure steady ion mobility proposed by Lieberman,combined with the fluid motion equation which described the continuous ion flux and Boltzmann relation of electron,the low-pressure non-steady diffusion fluid model is established, the effect of plasma diffusion on the sheath expansion, plasma recovery behavior and the effect of duty cycle on the ion implantation dose were studied. Calculating plasma density1010ions cm-3, electron temperature8eV, negative voltage pulses steady value-2kV, pulse width10μs, plasma source radius2.0cm, processing pressure10-1Pa, low-energy ion implanting the inner surface of tube with6.0cm radius, the non-steady diffusion of plasma can promote the sheath expansion, and the sheath size increased about0.31cm from1.96cm at the end of the pulse; high electron temperature and low processing pressure accelerate the plasma recovery process, which recovers to95%of the steady state just1.3μs after the end of the pulse, at2.8μs there is an overshoot phenomenon and after10.0μs the recovery gradually tends to steady state; the effect of duty cycle on the ion implantation energy is little, the duty cycle higher than0.8results in the plasma incomplete recovery, but high duty cycle can increase the ion implantation efficiency substantially. When the duty cycle is0.3, the average implanted ion current density is only0.86×10-4A/cm2, but when the duty cycle is0.9, the average implanted ion current density is up to2.60×10-4A/cm2. The duty cycle of0.9can provide the inner surface of the tube an ultrahigh ion implantation dose of5.8×1019ions cm-2during10h modification time. For the inner surface modification process by PBLEII, increasing the duty cycle of negative voltage pulses is an effective approach to increase the ion implantation dose.
引文
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