Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

  • Upload
    desc82

  • View
    218

  • Download
    0

Embed Size (px)

Citation preview

  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    1/9

    IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 31, NO. 4, AUGUST 2003 495

    Computational Study of Capacitively CoupledHigh-Pressure Glow Discharges in Helium

    Xiaohui Yuan and Laxminarayan L. Raja

    Abstract The structure of a capacitively coupled high-pressureglow (HPG) discharge in high-purity helium is investigated using adetailed one-dimensional modeling approach. Impurity effects aremodeled using trace amounts of nitrogen gas in helium. Averageelectrontemperaturesand densitiesfor the HPGdischargeare sim-ilar to their low-pressure counterpart. Helium-dimer ions domi-nate the discharge structure for sufficiently high-current densities,but model impurity nitrogen ions are found to be dominant forlow-discharge currents. Helium dimer metastable atoms are foundto be the dominant metastable species in the discharge. The highcollisionality of the HPG plasma results in significant discharge po-tential drop across the bulk plasma region, electron Joule heatingin the bulk plasma, and electron elastic collisional losses. High col-lisionality also results in very lowion-impact energies of order 1 eVat the electrode surfaces.

    Index Terms High-pressure glow (HPG) discharge, compu-tational modeling, capacitively coupled helium plasma, plasmaimpurity effects.

    I. INTRODUCTION

    L ARGE-VOLUME, high-pressure glow (HPG) dischargesare a class of electrical discharges characterized by stableand highly nonequilibrium glow plasmas that generated andsustained at pressures as high as one atmosphere [ 1][7].HPG discharge plasmas operate in a distinctive regime of plasma parameter space, where the plasma properties resemble alow-pressure glow plasmas, but at significantly higher pressureconditions. HPG discharges have traditionally been used forgas laser [ 8], [9] and combustion [ 10] applications, but there issignificant resurgence in HPG discharge research kindled bynew approaches to generating HPG plasmas and applicationsfor the same. The ability to dispense with vacuum systems havefacilitated the use of HPG discharges in etching and depositionof thin films [ 1], [11][13], surface modification [ 14], ozonegeneration [ 15], biosterilization [ 16], and as reflectors andabsorbers of electromagnetic radiation [ 17], [18].

    The novelty of HPG plasma phenomena is in the stable,large-volume, nonequilibrium characteristics at high pressures.

    Stability of a large-volume, self-sustained discharge dependsprincipally on the current density through the discharge.Above a certain threshold current density (typically of order50 mA/cm ), instabilities develop which leads to constriction

    Manuscript received November 1, 2002; revised February 22, 2003. Thiswork was supported by the National Science Foundation (NSF) under an NSF-CAREER Award (CTS-0 221 557).

    The authors are with the Department of Aerospace Engineering and Engi-neering Mechanics, The University of Texas at Austin, Austin, TX 78712 USA(e-mail: [email protected]).

    Digital Object Identifier 10.1109/TPS.2003.815479

    of the discharge volume and significant thermal heating of gas to form filamentary or arc plasmas. This phenomena iscalled the glow-to-arc transition. Pressure scaling relationshipsfor low-pressure glow discharges dictate that for a fixed totalcurrent the discharge current densities increase with increasingpressures [ 19]. Above a certain pressure (typically 10 torr),the current densities can exceed the threshold current densitiesfor instabilities to develop, resulting in a glow-to-arc transition.

    Traditional HPG discharge concepts rely on techniques thatlimit discharge current densities from exceeding the thresholdvalues for discharge stability [ 4]. For example, in dc HPG dis-

    charges, the cathode can be segmented into small sections andeach section individually ballasted with a large resistance tolimit the local current density to values below the threshold[8]. The same concept can be extended to nonsegmented cath-odesmadeof high-resistivity materials [ 20]. High gas-flow ratesthrough the discharge have also been used successfully to limitthe effect of instabilities [ 21]. Another approach has been tooperate HPG discharges in the pulsed mode with peak currentdensities that exceed the threshold but with pulse durations thatare short compared to time scales for growth of instabilities[22]. Other approaches that avoid electrodes altogether, suchas microwave-driven large-volume HPG discharges in the sur-face-wave mode, have also been proposed [ 23].

    In a relatively recent development, Kanazawa et al. [1]have reported a dielectric-barrier concept for HPG plasmageneration. A dielectric barrier covers one or both electrodesof a parallel-plate discharge, which are driven by a low-fre-quency ( 150 kHz), high-voltage ( 1 kV) power source.Highly stable, large-volume, nonequilibrium HPG plasmas aregenerated in this configuration. The dielectric barrier servesto trap charge on the surface during each half cycle, which,in turn, creates a surface-charge-induced field that opposesthe applied field. The plasma is thereby extinguished beforecurrent densities reach very high values. The overall effect of the dielectric barrier is to create a plasma pulse during eachhalf cycle [ 6], [7]. Another concept reported recently uses aparallel-plate electrode configuration without dielectric barrier,but driven at much higher radio-frequencies of order 10 MHz[5], [24], [25]. The discharge can be classified as a capacitivelycoupled HPG discharge and is generated in a closed spaceconfiguration with interelectrode spacing of a few millimetersat most.

    Despite significant interest, our current understanding of HPG phenomena remains incomplete. Recent computationalmodeling studies have begun to reveal some preliminaryinsights into HPG phenomena in both dielectric barrier [ 6] aswell as capacitively coupled configurations [ 26]. However,

    0093-3813/03$17.00 2003 IEEE

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    2/9

    496 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 31, NO. 4, AUGUST 2003

    a detailed understanding of the plasma dynamics, dominantphysical and chemical mechanisms, and structure of HPGdischarges is missing. We have previously reported a com-putational study of capacitively coupled HPG discharges anddescribed the role of trace impurities in such large-volume HPGplasmas [ 27]. In this study, we present a detailed computationalinvestigation of the structure and dynamics of capacitively

    coupled HPG discharges in pure helium. The presentation inthis paper is as follows. Section II presents a brief descriptionof the model, followed by results and discussions in Section III,and a summary with conclusions in Section IV.

    II. MODEL DESCRIPTION

    A. Governing Equations

    The computational model uses a one-dimensional (1-D) con-tinuum multifluid description of the plasma with individual con-tinuity equations describing the concentration of each chemicalspecies in the plasma, a current continuity equation for the elec-tric potential, and an electron energy equation to describe the

    electron temperature in the discharge. The modeling approachis similar to several other models reported in the literature (see[28] for an overview) and is described briefly in the following.

    The species continuity is given by

    (1)

    where is the number of a species, is the species fluxdensity, is the homogeneous production/destruction rateof species through gas phase reactions, and is the totalnumber of charged and neutral gas species in the system. and

    are the time and interelectrode axial distance, respectively.The electric potential in discharge is described by specifyingtotal current density through the discharge as

    (2)

    where is the electric potential, is the unit charge, andis the species charge number. The electron energy equation isgiven as

    (3)

    where and are the electron temperature and gas tempera-tures, respectively, is the electron thermal flux, is theenergy lost per electron in an inelastic collision event describedby gas-reaction , is the rate of progress of reaction , and iselectron momentum transfer collision frequency with the back-ground gas. and are the molecular masses of the elec-tron and dominant background species, respectively and isthe Boltzmann constant. The collision frequency of a speciesis evaluated as

    (4)

    where is the number density of the background species,is an effective molecular speed of the species, and is themomentum transfer collision cross section of the species withthe dominant background.

    Closure of the previous system of equations is achieved usingthe drift-diffusion approximation for the species number flux

    (5)

    and a Fouriers law approximation for the electron thermal flux

    (6)

    The species diffusion coefficients are evaluated as, species mobilities as ,

    and the electron thermal conductivity as .

    B. Boundary Conditions

    The boundary conditions imposed are as follows. Fluxboundary conditions are imposed for all species densities at theelectrodes. The electron and product neutral species fluxes aredetermined using a kinetically limited Maxwellian flux condi-tion as , where the signcorrespond to the lower and upper electrodes, respectively. Theions are assumed to be mobility limited at the boundaries andtheir boundary fluxes are specified as . Allmetastable species and ions are assumed to quench or neutralizeat the electrode surfaces and return back to the interelectrodespace as stable neutral species. The electron temperatures arefixed at the surface at 0.5 eV and secondary electron emission

    effects are ignored. We have performed sensitivity studies toconfirm that the assumptions of a fixed electron temperature atthe electrodes and zero secondary electron emission have nosignificant effect on the solutions.

    C. Plasma Chemistry

    The HPG plasma reaction mechanism for the high-purity he-lium includes pure helium and impurity species and their reac-tions. Our previous work has shown the importance of includingtheeffects of even trace amounts of impurity species in themod-eling of noble gas HPG plasma phenomena [ 27]. Since the exactcomposition of impurity species in the discharge is unknown,we have used nitrogen as a model impurity in the simulations.The reaction mechanism is shown in Table I and is compliedfrom several literature sources [ 29][32].

    D. Transport Properties

    Table II presents the transport properties of the plasmaspecies. The properties are given in terms of reduced diffusioncoefficients and mobilities and are defined in terms of

    , and , respectively, withbeing the discharge pressure in torr. These properties have beencomplied from literature data [ 19], [35], [36], and are evaluatedassuming species transport in a helium background gas at atemperature of 393 K.

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    3/9

    YUAN AND RAJA: COMPUTATIONAL STUDY OF CAPACITIVELY COUPLED HPG DISCHARGES IN HELIUM 497

    TABLE IREACTION MECHANISM FOR HIGHPRESSURE HELIUM GLOW PLASMA WITH NITROGEN IMPURITY

    TABLE IIREDUCED DIFFUSION COEFFICIENTS AND MOBILITIES OF SPECIES IN A

    BACKGROUND HELIUM GAS

    III. RESULTS AND DISCUSSIONS

    Computational results presented here are validated using datafrom recent capacitively coupled HPG discharge experimentalstudies by Park et al. [25]. The experiments were conductedin a parallel-plate discharge configuration with stagnant (non-flowing), high-purity helium as the working gas. The stagnantgas environment allows accurate modeling using the 1-Dapproach. Discharge characteristics for varying interelectrodespacing and pressures, at a fixed frequency of 13.56 MHz aresimulated in this study.

    As mentioned in our previous paper [ 27], trace impuritiesplay an important role in determing the structure and dy-namics of noble gas HPG discharges and their effect must be

    included to predict even global discharge parameters such asthe voltagecurrent ( VI ) characteristics. The main effect of the trace impurities is to significantly decrease the differential

    impedance of the discharge compared to pure helium. Theexact concentration of model impurity is, therefore, a modelparameter that is determined to best match experimental results.We have found that model nitrogen impurity with an initialimpurity mole fraction of 5 10 (99.99995% or 0.5 ppm)in pure helium provides best comparison to experimental data[27]. This concentration is fixed for all simulation in our studyand is within the rate impurity concentration of 99.9995% forthe helium gas used in the experiments. Order-of-magnitudeestimates indicate that gas heating under discharge conditionsare not significant enough to cause a large temperature rise. Inour study, the gas temperature is assumed fixed at 393 K and isthe same as the experimentally measured gas temperatures [ 25].

    We first provide validation of the modeling approach by di-rect comparison between experimental data and our simulationresults for VI characteristics of the discharge. Fig. 1 showsroot-mean-square (rms) VI characteristics for varying inter-electrode distances of 1.6, 2.4, and 3.2 mm at a fixed dischargepressure of 600 torr. The same characteristics for varying pres-sures of 300, 450, and 600 torr at a fixed interelectrode distanceof 2.4 mm is presented in Fig. 2. All experimental VI curvesshow an initial prebreakdown (no discharge) stage with linearrise in the voltage followed by a HPG stage where the voltageincreases slowly for an increase in the current. For higher cur-rent densities, the voltage becomes relatively independent of thecurrent through the discharge. The differential impedance of the

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    4/9

    498 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 31, NO. 4, AUGUST 2003

    Fig. 1. Comparison of experimental and simulated rms VI characteristics forvarying interelectrode distances of 1.6, 2.4, and, 3.2 mm and a fixed pressureof 600 torr. The RF frequency is 13.56 MHz for all cases. Circle symbolscorrespond to 1.6, triangles are 2.4, and rectangles are at 3.2 mm. Simulationresults are connected by a line.

    Fig. 2. Comparison of experimental and simulated rms VI characteristics forvarying discharge pressures of 300, 450, 600 torr, and a fixed interelectrodedistance of 2.4 mm. The RF frequency is 13.56 MHz for all cases. Circlesymbols correspond 300, triangles are 450, and rectangles are at 600 torr.Simulation results are connected by a line.

    HPG discharge is, therefore, small for low-current densities andnearly zero for high-current densities. HPG discharge voltagesincrease with increasing interelectrode distance for a fixed pres-sure and increase with increasing pressures for a fixed inter-electrode distance. The maximum current densities for whichthe experimental data are shown correspond to threshold cur-rent densities for glow-to-arc transition. The model predicts allimportant features of the experimental data with good predic-tions of the experimental voltages at the high-current densities.

    The voltage is underpredicted at low-current densities but thetrends are captured adequately. Importantly, the low differentialimpedance at low-current densities followed by the near-zerodifferential impedance at the high-current densitiesare observedin the model results. We must, however, emphasize that themodel does notrepresent thephysics of thedischarge adequatelyto capture the breakdown and glow-to-arc transition limits.

    Fig. 3 shows the voltage- and current-density waveforms fora 600 torr discharge, with a 2.4-mm interelectrode spacing anda 21.2 mA/cm rms current density. The waveforms show asmooth and near-sinusoidal voltage characteristic for the im-posed sinusoidal current. The current is also found to lead thevoltage waveform by 35.7 . These model results are consistent

    Fig. 3. Simulated voltage and current density waveforms for a 600-torrdischarge with 2.4-mm interelectrode spacing, 13.56-MHz RF frequency, and21.2-mA/cm rms current density.

    Fig. 4. Simulated potential profiles at four times instances during an RFcycle for a 600-torr discharge with 2.4-mm interelectrode spacing, 13.56-MHzRF frequency, and 21.2-mA/cm rms current density. The fractional time0 corresponds to a positive maximum phase of the discharge current, 0.25corresponds to zero current, 0.5 corresponds to the negative maximum phaseof the discharge current, and 0.75 to the subsequent zero current.

    withexperimentaldata, wheresmooth and nearly sinusoidal VI waveforms are observed under HPG conditions, especially atlow- and intermediate-current densities [ 25].

    Fig. 4 shows the interelectrode electric potential profiles forthe same discharge parameters as in Fig. 3. Distinct regionscorresponding to the electrode sheaths and a bulk plasma inbetween them, can be identified. Large potential drops areobserved at the sheaths at cycle fractional times of 0.25 and0.75 while large drops are observed through the bulk plasmaat fractional times of 0 and 0.5. The cycle fractional timesof 0.25 and 0.75 correspond to the zero current phases of

    the cycle, while fractional times of 0 and 0.5 correspond tothe maximum current phases of the cycle. These dischargepotential profiles show significant differences compared toclassical low-pressure capacitively coupled glow discharges,where the discharge potential drops occuralmost entirely acrossthe sheaths at all times during an RF cycle. The large bulk plasma potential drop for the HPG discharge at the maximumcurrent phases is a result of the high pressures which resultsin significant resistivity of the bulk plasma. The maximumelectric field strength predicted in the sheath region of the HPGdischarge is of order 4 kV/cm which is somewhat higher thantypical field strengths ( 0.5 kV/cm) observed in the sheathsof low-pressure capacitively coupled discharges [ 31], [33].

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    5/9

    YUAN AND RAJA: COMPUTATIONAL STUDY OF CAPACITIVELY COUPLED HPG DISCHARGES IN HELIUM 499

    Fig. 5. Spatial profiles of important discharge parameters. The dischargeoperating conditions are the same as in Fig. 4. The top panel shows thetime-averaged electron temperature and number densities. The center panelshows the dominant ion densities and the bottom panel shows the neutralspecies densities.

    Spatial profiles of time-averaged electron temperature andspecies number densities are shown in Fig. 5. The dischargeoperating conditions are the same as in Fig. 4. The top panelshows time-averaged profiles of the electron temperature and

    electron number densities. The average temperature is nearlyuniform in the bulk plasma (about 1 eV) but rises to peak valuesof about 2.5 eV within the sheaths. The average electron densityis a maximum at the center of the discharge and drops towardthe electrodes. The peak calculated electron density is about1.8 10 m at the center of the discharge and is close to theexperimental estimate of 3 10 m [ 25]. A small hump inthe electron density profile is observed inside the sheaths and isa consequence of significant volumetric production of electronsthrough plasma reactions in the sheaths. This phenomena mustbe contrasted with low-pressure glow discharge sheaths whereeffect of plasma chemistry is negligible and charge generationis mostly confined to the sheath-bulk plasma interface and bulk

    plasma region [ 31], [33], [34]. The center panel shows time-av-eraged ion density profiles in the discharge. The ion densitiesexperience negligible modulation during an RF cycle owing totheir heavier mass, although relatively small modulations arenoticed for the helium ions within the sheaths. The dominantion in the bulk plasma is He , while the impurity ion N domi-nates in the sheath region. N ion density profile resembles theHe ions with a maximum at the center of the discharge andmuch lower values in the sheaths. He ion densities are neg-ligible throughout the discharge. The ion density profiles indi-cate that He and N ions are generated by reactions in the bulk plasmaor thesheath-bulkplasma interfaceregions while theNions aregenerated predominantly within the sheath regions. The

    Fig. 6. Time-averaged contributions of gas-phase reaction pathways tothe generation/destruction of electrons in the HPG discharge. The dischargeoperating conditions are the same as in Fig. 4.

    neutral species profiles are shown in the bottom panel. Both thehelium metastable species He and He have peaks within thesheaths, indicating significant volumetric production of thesespecies inside the sheath regions. The helium metastable pro-files have a minimum at the center of the discharge owing to netvolumetric destruction in the bulk plasma. The metastable den-sities drop close to the electrodes owing to surface quenchingeffects. The nitrogen atom N shows a peak at the center of thedischarge and drop toward the electrodes. The nitrogen (impu-rity) molecules N are depleted at the center of the dischargeand are regenerated at the two electrodes by surface neutral-ization of nitrogen ions and recombination of N radicals. TheHe background species density is nearly uniform throughout thedischarge and has a value of 1.47 10 m .

    The previous spatial profiles of important species in theplasma are established by the combined effect of gas-phaseplasma reactions, transport, and surface reactions at the elec-trodes. The time-averaged contributions of the gas-reaction

    pathways to the productions/destruction of electrons in thedischarge are presented in Fig. 6. The discharge operatingconditions are the same as in Fig. 4. The figure shows ratesof 11 reactions (see Table I) that contribute to the electrondensity balance. The reactions with highest contribution tothe volumetric production rate of electrons are shown in thetop panel. Reaction , which is the Penning ionization of N by metastable He , is the dominant reaction for electronproduction and plays an important role only within the sheathswhere N densities are high. The second most important con-tribution comes from reaction , which is the electron impactionization of the He background atoms. Again the contributionof this reaction is dominant in the sheaths where the electron

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    6/9

    500 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 31, NO. 4, AUGUST 2003

    Fig. 7. Time-averaged contributions of Joule heating, and elastic and inelasticcollisions to the electron energy balance in the discharge. The dischargeoperating conditions are the same as in Fig. 4.

    temperatures are high. The center and bottom panels show thatreactions (Penning ionization of N by metastable He ),

    (stepwise ionization of He ), (electron impact ioniza-tion of N), (stepwise ionization of He ), and (electronimpact ionization of N ) also play a relatively minor role in theelectron production inside the sheaths. In the bulk plasma, thedominant contributors to electron production are , followedby . The bottom panel shows that the electrons are alsoconsumed within the discharge by reactions (dissociativerecombination of N ) and (dissociative recombination of He ). The remaining electrons are consumed at the electrodes.

    Fig. 6 provides a vivid picture of how the impurity species(N ) alters the charge balance in a noble gas HPG dischargeby participating in Penning ionizations reactions within thesheaths. The figure also points to another important distictionbetween low-pressure glow and HPG discharges. Unlike

    low-pressure capacitively coupled discharges where chargeproduction is confined mostly to the sheath-bulk plasmainterface region [ 31], [33], [34], the charge production inHPG discharges is distributed throughout the discharge and inparticular is very high within the sheath regions.

    The time-averaged contributions of volumetric source/sink terms that contribute to the electron energy balance in the dis-charge are shown in Fig. 7. These include Joule heating, in-elastic collisional loss/gain, and elastic collisional loss terms.These are the third, fourth, and fifth terms in (3), respectively.Joule heating is the principal source of electron heating in thedischarge and is dominant in the bulk plasma as well as thesheath-bulk plasma interface region. The main volumetric loss

    of electron energy comes from elastic collisions of thehigh-tem-perature electrons with the low-temperature background heavyspecies. Inelastic collisions contribute to a net loss of electronenergy although themagnitude of theinelastic loss is small com-pared to the elastic collisional loss of electron energy. Fig. 7 alsopoints to important differences in the mechanisms of electronenergy balance in HPG discharges and low-pressure glow dis-charges. In capacitively coupled low-pressure glow discharges,Joule heating is largely confined to thesheath-bulkplasmainter-face regions where electric field strengths are high and electronparticle fluxes are significant [ 33], [34]. In the capacitively cou-pled HPG discharge, however, electric fieldstrengthsarehigh inthe bulk plasma as well as the sheaths and, hence, Joule heating

    Fig. 8. Dependence of time-averaged electron density profiles for varyingdischarge parameters. The top panel shows variation with rms current densityfor fixed pressure of 600 torr and 2.4-mm interelectode gap. The middle panelshows variations with pressure for a fixed rms current density of 21.2 mA/cmand 2.4-mm interelectode gap. The bottom panel shows variations withinterelectrode gap for a fixed pressure of 600 torr and rms current density of 21.2 mA/cm . The RF frequency is 13.56 MHz for all cases. The units for eachparameter varied are indicated in brackets.

    is distributed throughout the discharge, except near the electrodewhere electron densities are low. Another major difference be-tween low-pressure and HPG discharges is the contribution of

    elastic collisional loss terms. Elastic collisional loss to the back-ground gas is negligible in most low-pressure glow dischargesand is often neglected in the modeling of such discharges [ 28].However, elastic collisions are the dominant volumetric electronenergy loss mechanism in HPG discharges.

    The effect of changes in discharge operating parameters isdiscussed next. Fig. 8 shows the time-averaged electron den-sity profiles for changes in the rms current density, pressure,and interelectrode gap. The magnitude of the current densitiesthrough the discharge has a large impact on the discharge struc-ture. The electron densities increase for increasing current den-sities. In addition, electron production due to Penning ionizationreactions within the sheaths depends significantly on the current

    densities through the discharge. For the lowest current densitycase shown (8.5 mA/cm ), theelectron production in thesheathsis negligible compared to the higher current density cases. This,in turn, manifests itself as an increasingly prominent hump inthe density profiles within the sheath regions for increasing cur-rent densities. As shown in the center panel, the electron den-sities are nearly unchanged for changes in discharge pressure,indicating that under high-pressure conditions, the magnitudeof the discharge pressure itself is relatively unimportant in de-termining theglobalcharacteristicsof an HPG plasma. From thebottom panel it is seen that changes in the gap distance resultsin a relatively small increase in the maximum electron numberdensities at the center of the discharge. Since the sheath thick-

    http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    7/9

    YUAN AND RAJA: COMPUTATIONAL STUDY OF CAPACITIVELY COUPLED HPG DISCHARGES IN HELIUM 501

    Fig. 9. Dependence of the time-averaged electron temperatures for varyingdischarge parameters. The parameters varied in each panel are the same as inFig. 8.

    ness remains relatively constant for all gap lengths, the maineffect of increasing the gap length is the increase in the lengthof the bulk plasma region.

    The effect of varying discharge operating parameters on thetime-averaged electron temperature profiles is shown in Fig. 9.The toppanel shows that with theexception of thelowest currentdensity case (8.5 mA/cm ), the electron temperatures are rela-tively independent of the magnitude of the current flow throughthedischarge. Forthe low-currentdensity case, theaverageelec-tron temperature in thebulk plasma is about 0.2 eV, which is sig-nificantly lower than the 1-eV average temperature for the othercases. As in the case of electron densities, the electron tempera-tures are relatively independent of the discharge pressures. Also,variations in the gap length results in a longer bulk plasma re-gion with negligible change in magnitudes of the bulk plasmatemperature and peak sheath temperature.

    Results from both Figs. 8 and 9 indicate that the rms currentdensity through the discharge has the most significant effect onthe HPG discharge properties. In particular, two distinct regimes

    in thecurrentdensity canbe identified;one beingthe low-currentdensity regime and the other the intermediate to high-currentdensity regime. These two regimes were identified in our earlierdiscussion on the discharge VI characteristics, as regimeswith low-differential impedance (low-current densities) andnear-zero differential impedance (intermediate-to-high currentdensities). Further insights into the discharge structure in thesecurrent regimes can be obtained from Fig. 10, where thetime-averaged profiles of all ions in the discharge are plottedat the three rms currents densities for a fixed pressure of 600 torr and a gap of 2.4 mm. The intermediate (21.2 mA/cm )and high-current density (31.8 mA/cm ) cases are characterizedby He as the dominant ion in the bulk plasma region and N

    Fig. 10. Dependence of the time-averaged ion density profiles on the currentdensities through the discharge. The pressure is fixed at 600 torr, the RFfrequency is 13.56 MHz, and the gap distance is 2.4 mm. The numbers againsteach curve indicates the the rms current density in mA/cm .

    as the dominant ion in the sheath regions. Somewhat lower Nions are also observed in the bulk-plasma region. However,in the low-current density case (8.5 mA/cm ), the dischargestructure swithes to a different regime where the impurity ionN is the only dominant ion in the discharge with all other

    ion densities being negligible. He ions are negligible for allcases.An detailed analysis of the gas reaction pathways for the

    low-current density case compared to the intermediate andhigh-current density cases reveals reasons for the switch inthe dominant bulk plasma ion species at low-current densi-ties compared to intermediate and high-current densities. Therelatively low bulk plasma electron temperatures of 0.2 eV inthe low-current density case causes Penning ionization of theimpurity molecule N (reactions and ) to dominatethe overall ionization rate when compared to direct or step-wise ionization of helium (reactions or ). This is owingto the fact that direct and stepwise ionization of helium are

    activated processes and require higher electron temperaturesfor the corresponding rates to be high. As a consequence, Nions are the dominant ion species at the low current densities.At higher current densities, the plasma electron temperaturesare higher, causing the direct and stepwise ionization of he-lium to dominate the plasma ionization mechanism. He ionsproduced thereby, are rapidly converted to He ions throughthree-body reaction , resulting in dominant He in the bulk plasma for the intermediate- to high-current density cases.

    Finally, the ion impact energy distribution functions (IEDF)at one of the electrodes for discharge pressures of 600 and300 torr are presented in Fig. 11. The IEDF is defined as thefractional flux of each type of ions impacting the surface at a

  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    8/9

    502 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 31, NO. 4, AUGUST 2003

    Fig. 11. Ion impact energy distribution functions for each ion speciesimpacting an electrode. The discharge parameters correspond to 2.4-mminterelectrode gap, 13.56-MHz RF frequency, and 21.2-mA/cm rms currentdensity. The top panel shows results for 600 torr and the bottom panel for300-torr discharge pressures.

    given impact energy, per unit impact energy. The IEDFs forall ions are bimodal with a peak at the minimum energy of ionimpact and another peak at the maximum energy of ion impact.The bimodal IEDF is also observed for RF biased surfacesin low-pressure glow discharges. For the HPG discharge, theminimum energy peaks correspond to near-zero ion impactenergies for all ions, while the maximum energy peak variessignificantly depending on the type of ion and the pressure. Theion impact energy distribution is found to be widest for the N

    ions, followed by N , He , and He in order of decreasingdistribution widths. The maximum ion impact energy at600 torr is about 1 eV for the N ions and about 0.05 eV for theHe ions. The corresponding maximum ion impact energies at300 torr are about 3.6 eV for N ions and 0.2 eV for He ions.

    The previous ion impact energy distribution trends are con-trary to trends observed for RF biased surfaces in low-pressureglow discharges. In low-pressure glow discharges the distribu-tion widths increase with decreasing ion mass [ 37][39] whilein the HPG discharge the widths decrease with decreasing ionmass. For low-pressure glow discharges, the sheaths are weaklycollisional or collisionless which causes ion transport in thesheath to be dominated by inertial effects resulting in the IEDF

    widths being inversely related to the ion mass. In HPG dis-charges, the sheaths are highly collisional and the ion transportdepends largely on the electric-field-induced species mobility.Ions with higher mobility are able to follow the sheath electricfield oscillation moreclosely and henceexperience widerIEDFsat the electrode surface. Lower mobility ions are much moresluggish in their response to sheath electric field oscillations,which results in a narrower IEDFs. In a helium background gas,the ions N , N , He , and He ions have decreasing mobilityin that order (see Table II) and, hence, their ion impact energydistributionshave correspondingly narrowerdistributions. A de-crease in the discharge pressure results in an overall increase inthemobility of allions, which results in wider distribution forall

    ions. For example, at 300 torr, the maximum ion impact energyof N increases to about 3.7 eV compared to 1 eV at 600 torr.

    IV. CONCLUSION

    We have presented a detailed computational study of ca-pacitively coupled, HPG discharges in high purity helium. A

    1-D, self-consistent, continuum plasma model is developed andused. Small concentrations of a model nitrogen impurity inpure helium (5 10 in mole fraction or 0.5 ppm) is requiredto model discharge properties accurately. The model predictsthe experimental VI characteristics for a range of pressuresand gap distances. The discharge structure consists of a bulk plasma region and sheath regions adjacent to the electrodes.The predicted average electron temperatures of order 1 eV andelectron number densities of order 10 cm are comparable tothose found in most low-pressure glow discharges. The electrontemperatures are relatively independent of the current densitythrough the discharge as well as discharge pressures, except forlow-current densities where the temperature drops significantly.

    The electron temperatures depend largely on Joule heating inthe bulk plasma and the sheath-plasma interface regions as wellas electron energy loss by elastic collisions with colder heavyspecies. This contrasts with low-pressure capacitively coupledglow discharges where elastic collision losses are negligibleand Joule heating is dominant only in the plasma-sheath in-terface region. The plasma electron density depends stronglyon the current density through the discharge but is relativelyindependent of the discharge pressure. The ion concentrationin the discharge is dominated by dimer helium ions He in thebulk plasma and impurity N ions in the sheaths. However,at low-current densities the impurity ions dominate almost theentire discharge structure. The dimer helium metastables Heare observed to be the dominant metastable species in thedischarge with densities of order 10 cm . Owing to highlycollisional sheaths, the ion-impact energies at the electrodesare found to range from near-zero values to a maximum of afew electronvolts. These energies are very low compared tolow-pressure glow discharges where ion impact energies canrange from order 10 to a few 100 eV.

    REFERENCES[1] S. Kanazawa, M. Kogoma, T. Moriwaki, and S. Okazaki, Stable glow

    plasma at atmospheric pressure, J. Phys. D, Appl. Phys. , vol. 21, pp.838840, 1988.

    [2] S. Okazaki, M. Kogoma, M. Uehara, and Y. Kimura, Appearance of

    stable glow discharge in air, argon, oxygen, and nitrogen at atmosphericpressure using a 50 Hz source, J. Phys. D, Appl. Phys. , vol. 26, pp.889892, 1993.

    [3] M. Moisan, Z. Zakrzewski, R. Etmadi, and J. C. Rostaing, Multitudesurface-wave discharges for increased gas throughput at atmosphericpressure, J. Appl. Phys. , vol. 83, pp. 56915701, 1998.

    [4] E. E. Kunhardt, Generation of large-volume, atmospheric-pressure,nonequilibrium plasmas, IEEE Trans. Plasma Sci. , vol. 28, pp.189200, Feb. 2000.

    [5] A. Schutze, J. Y. Jeong, S. E. Babayan, J. Park, G. S. Selwyn, and R.F. Hicks, The atmospheric-pressure plasma jet: A review and com-parison to other plasma source, IEEE Trans. Plasma Sci. , vol. 26, pp.16851694, Dec. 1998.

    [6] F. Massines, A. Rabehi, P. Decomps, R. Ben Gadri, P. Segur, and C.Mayoux, Experimental and theoretical study of a glow discharge at at-mospheric pressure controlled by dielectric barrier, J. Appl. Phys. , vol.83, pp. 29502957, 1998.

    http://-/?-http://-/?-http://-/?-http://-/?-
  • 8/10/2019 Computational Study of Capacitively Coupled High-Pressure Glow Discharges in Helium

    9/9

    YUAN AND RAJA: COMPUTATIONAL STUDY OF CAPACITIVELY COUPLED HPG DISCHARGES IN HELIUM 503

    [7] L. Mangolini, K. Orlov, U. Kortshagen, J. Heberlein, and U. Ko-gelschatz, Radial structure of a low-frequency atmospheric-pressureglow discharge in helium, Appl. Phys. Lett. , vol. 80, pp. 17221724,2002.

    [8] A. J. Beaulieu, Transverselyexcited atmospheric pressure CO lasers, Appl. Phys. Lett. , vol. 16, pp. 504505, 1970.

    [9] M. J. Kushner, Microarcs as a termination mechanism of optical pulsesin electric-discharge-excited KrF excimer lasers, IEEE Trans. PlasmaSci. , vol. 19, pp. 387399, Apr. 1991.

    [10] T. Peterson and R. C. Brown, Simulation of electric field effects in pre-mixed methane flames, Combust. Flame , vol. 94, pp. 433448, 1993.[11] J. Y. Jeong, S. E. Babayan, A. Schutze, V. J. Tu, J. Park, I. Henins, R. F.

    Hicks, and G. S. Selwyn, Etching polyimide with a nonequilibrium at-mospheric-pressure plasma jet, J. Vac. Sci. Technol. A, Vac. Surf. Films ,vol. 17, pp. 25812585, 1999.

    [12] Y. Sawada, S. Ogawa, and M. Kogoma, Synthesis of plasma-polymer-ized tetraethoxysilane and hexamethyldisiloxane films prepared by at-mospheric pressure glow discharge, J. Phys. D, Appl. Phys. , vol. 28,pp. 16611669, 1995.

    [13] N. Gherardi, S. Martin, and F. Massines, A new approach to SiOdeposit using a N -SiH -N O glow dielectric barrier-controlled dis-charge at atmospheric pressure, J. Phys. D, Appl. Phys. , vol. 33, pp.L104L108, 2000.

    [14] F. Massines and G. Gouda, A comparison of polypropylene-surfacetreatment by filamentary, homogeneous and glow discharges in he-lium at atmospheric pressure, J. Phys. D, Appl. Phys. , vol. 31, pp.

    34113420, 1998.[15] M. Kogoma and S. Okazaki, Raising of ozone formation efficiency in ahomogeneous glow discharge plasma at atmospheric pressure, J. Phys. D, Appl. Phys. , vol. 24, pp. 19851987, 1994.

    [16] J. R. Roth, D. M. Sherman, R. B. Gadri, F. Karakaya, Z. Chen, T. C.Montie, K. Kelly-Wintenberg, and P. P.-Y. Tsai, A remote exposurereactor (RER) for plasm processing and sterilization by plasma activespecies ate one atmosphere, IEEE Trans. Plasma Sci. , vol. 28, pp.5663, Feb. 2000.

    [17] R. J. Vidmar, On the use of atmopheric pressure plasmas as electro-magnetic reflectors and absorbers, IEEE Trans. Plasma Sci. , vol. 19,pp. 733741, Aug. 1990.

    [18] W. W. Destler, J. E. DeGrange, H. H. Fleischmann, J. Rodgers, andZ. Seglov, Experimental studies of high-power microwave reflection,transmission, and absorption from a plasma-covered plane conductingboundary, J. Appl. Phys. , vol. 69, pp. 63136318, 1991.

    [19] Yu. P. Raizer, Gas Discharge Physics . Berlin, Germany:

    Springer-Verlag, 1991.[20] P. D. Slade and A. Serafetinides, Stable discharge in an HF laser withinlarge electrode separation, IEEE J. Quantum Electron. , vol. QE-14, pp.321322, May 1978.

    [21] Yu. S. Akishev, A. A. Deryugin, V. B. Karalnik, I. V. Kochetov, A.P. Napartovich, and N. I. Trushkin, Numerical simulation and experi-mental studyof an atmospheric-pressure direct-current glowdischarge,Plasma Phys. Rep. , vol. 20, pp. 511524, 1994.

    [22] W. W. Byszewski, Diffuse discharges at high-current density, J. Appl.Phys. , vol. 66, pp. 103107, 1989.

    [23] M. Moisan, R. Pantel, J. Hubert, E. Bloyet, P. Leprince, J. Marec, andA. Ricard, Production and applications of microwave surface plasma atatmospheric pressure, J. Microwave Power , vol. 14, pp. 5761, 1979.

    [24] J. Park, I. Henins, H. W. Herrmann, and G. S. Selwyn, Gas breakdownin an atmospheric pressure radio-frequency capacitive plasma source, J. Appl. Phys. , vol. 89, pp. 1519, 2001.

    [25] J. Park, I. Henins, H. W. Hermann, G. S. Selwyn, and R. F. Hicks, Dis-

    charge phenomena of an atmospheric pressure radio-frequency capaci-tive plasma source, J. Appl. Phys. , vol. 89, pp. 2028, 2001.[26] J.Park,I. Henins, H.W. Hermann, G. S. Selwyn, J. Y. Jeong,R. F. Hicks,

    D. Shim, and C. S. Chang, An atmospheric pressure plasma source, Appl. Phys. Lett. , vol. 76, pp. 288290, 2000.

    [27] X. Yuan and L. L. Raja, Role of trace impurities in large-volume noblegas atmopheric-pressureglowdischarges, Appl. Phys. Lett. , vol.81, pp.814816, 2002.

    [28] T. R. Govindanand M. Meyyappan, One-dimensional modelingstudiesof the gaseous electronics conference RF reference cell, J. Res. Natl. Inst. Stand. Technol. , vol. 100, pp. 463472, 1995.

    [29] S. Rauf and M. J. Kushner, Dynamics of a coplanar-electrode plasmadisplay panel cell, J. Appl. Phys. , vol. 85, pp. 34603469, 1999.

    [30] J.W.Shonand M.J. Kushner, Excitation mechanismand gain modelingof the high-pressure atomic Ar laser in He/Ar mixtures, J. Appl. Phys. ,vol. 75, pp. 18831890, 1994.

    [31] T. J. Sommerer and M. J. Kushner, Numerical investigation of the ki-

    netics and chemistry of RF glow discharge plasmas sustained in He, N ,O , He/N /O , He/CF /O , and SiH /NH using a monte carlo-fluidhybrid model, J. Appl. Phys. , vol. 71, pp. 16541673, 1992.

    [32] C. O. Laux, L. Yu, D. M. Packan, R. J. Gessman, L. Pierrot, C. H.Kruger, and R. N. Zare, Ionization mechanisms in two-temperatureair plasmas, presented at the 30th AIAA Plasmadynamics and LasersConf. , Norfolk, VA, 1999, AIAA Paper 99-3476.

    [33] M. Surendra andD. B. Graves, Particles simulationsof radio-frequencyglow discharges, IEEE Trans. Plasma Sci. , vol. 19, pp. 144157, Apr.1991.

    [34] D. P. Lymberopoulos and D. J. Economou, Fluid simulations of glowdischarges: Effect of metastable atoms in argon, J. Appl. Phys. , vol. 73,pp. 36683679, 1993.

    [35] R. J. Kee, G. Dixon-Lewis, J. Warnatz, M. E. Coltrin, and J. A. Miller,A Fortran computer code package of gas-phase multicomponent trans-portproperties, Sandia Nat. Lab., Livermore, CA, Rep.SAND86-8246,1995.

    [36] H. W. Ellis,R. Y. Pai, E. W. McDaniel, E. A. Mason,and L. A. Viehland,Transport properties of gaseous ionsover a wide energy range, Atomic Data Nucl. Data Tables , vol. 17, pp. 177210, 1976.

    [37] M. S. Barnes, J. C. Forster, and J. H. Keller, Ion kinetics in low-pres-sure, electropositive, RF glow discharge sheaths, IEEE Trans. PlasmaSci. , vol. 19, pp. 240244, Apr. 1991.

    [38] P. A. Miller and M. E. Riley, Dynamics of collisionless RF plasmasheaths, J. Appl. Phys. , vol. 82, pp. 36893709, 1997.

    [39] L. L. Raja and M. Linne, Analytical model for ion angular distributionfunctions at RF biased surfaces with collisionless plasma sheaths, J. Appl. Phys. , vol. 93, pp. 70327040, 2003.

    Xiaohui Yuan received the B.S. degree in chemicalengineering from Tsinghua University, Beijing,China, in 1999, and is currently working toward thePh.D. degree.

    Laxminarayan L. Raja received the B.Tech. degreein aerospace engineering from the Indian Institute of Technology, Chennai, India, in 1990, the M.S.degreein nuclear engineering from Texas A&M University,College Station, in 1992, and the Ph.D. degree in me-

    chanical engineering from The Universityof Texas atAustin, in 1996.He is currently an Assistant Professorof aerospace

    engineering at The University of Texas at Austin. Hisresearch interests include glow-discharge plasmas,computational modeling and experimental studies

    of high-pressure glow discharges, materials processing discharges, and plasmapropulsion for spacecrafts.