BELEVTSEV A A，F(xiàn)IRSOV K N，KAZANTSEV S Yu，KONONOV I G，ZHANG Lai-ming

（1.Joint Institute for High Temperatures，Institute for High Energy Densities，Russian Academy of Sciences，Moscow 125412，Russia；2.Prokhorov General Physics Institute，Russian Academy of Sciences，Moscow 119991，Russia；3.State Key Laboratory of Laser Interaction with Mater，Changchun Institute of Optics，F(xiàn)ine Mechanics and Physics，Chinese Academy of Sciences，Changchun 130033，China）

Electron detachment instability and self-organization of gas discharge plasma in working mixtures of chemical non-chain HF（DF）lasers

BELEVTSEV A A1，F(xiàn)IRSOV K N2，KAZANTSEV S Yu2，KONONOV I G2，ZHANG Lai-ming3

（1.Joint Institute for High Temperatures，Institute for High Energy Densities，Russian Academy of Sciences，Moscow 125412，Russia；2.Prokhorov General Physics Institute，Russian Academy of Sciences，Moscow 119991，Russia；3.State Key Laboratory of Laser Interaction with Mater，Changchun Institute of Optics，F(xiàn)ine Mechanics and Physics，Chinese Academy of Sciences，Changchun 130033，China）

This paper reports on investigating the ionization instability in active media of electric discharge non-chain HF（DF）lasers due to electron impact detachment of electrons from negative ions.This instability has been triggered in large volumes of SF6-based mixtures，spatially separated from electrodes，through the gas heating by a pulsed CO2laser radiation.A self-organization phenomenon in a Self-sustained Volume Discharge（SSVD）on a laser-induced gas heating and resulting in formation of quasi-periodic plasma structures in the bulk of discharge gap is experimentally studied.Special attention is given to the evolution of these structures on changing the gas temperature and specific electric energy depositions.A plausible relation of the found selforganization effect to the electron detachment instability treated is discussed.Also suggested is the mechanism of moving a single plasma channel in working media of HF（DF）lasers owing to destruction of negative ions by electron impact.

HF（DF）laser；electron detachment instability；self-organization phenomenon；self-sustained volume discharge；plasma structure

1 Introduction

Ionization instability of Self-sustained Volume Discharge（SSVD）in SF6and its mixtures is of great interest in view of development of chemical non-chain HF（DF）lasers[1］.

Currently，a number of ionization instability mechanisms in electronegative gases are known.A general theoretical approach to the problem is developed in Ref.[2］.In Ref.[3］-[5］，the mechanisms are thoroughly considered of the ionization instability in working media of CO2lasers due to electron detachment from negative ions by neutral and electronically excited components.For excimer lasers，the instability mechanism arising from the electron impact dissociation of small electronegative admixtures（“burning away”of a halogen additive）has been studied in greater detail in Ref.[6］-[9］. The instability in SF6，according to Ref.[10］，may exclusively be caused by the stepwise ionization of SF6molecules.

A qualitatively new scenario of the ionization instability owing to electron detachment from negative ions by electron impact can be realized in strongly electronegative gases at intermediate pressures on the time scale of several tens of nanoseconds.For the first time，this problem was touched up in Ref.[11］，as applied to SSVD in SF6and its mixtures.The key idea is in the following.

In SF6-based mixtures at intermediate pressures and room temperatures，the best agreement between the calculated time dependences and the recorded SSVD voltage and current oscillograms，including a quasi-stationary phase（E/N≈（E/Ncr），is attained on taking βei≈kd（see below）.Here E is the electric field strength，N is the gas number density；βeiand kdare the rate constants for electron-ion dissociative recombination and the electron detachment of electrons from negative ions by electron impact；（E/ N）cris the critical reduced electric field.Under the conditions mentioned，the increase in the electron concentration due to destruction of negative ions by electron impact is practically compensated for their losses in a dissociative electron-ion recombination. The above-stated nonlinear mechanism of electron multiplication comes，therefore，to manifest itself only at significant unbalance between the rates βeiand kd，which is achieved either at strong gas heating or if E/N?（E/N）cr.Indeed，the rate constant βei～TgT-χe（χ＞0，Tgis the gas temperature，Te= 2〈ε〉/3 is the mean electron energy[12］decreases in both cases，while εdvalue can only increase.

The condition E/N?（E/N）crcan actually be realized in the vicinity of the tip of an incomplete channel growing from the cathode side.However，the ionization processes develop here only at the distances approaching the channel radius；hereupon great difficulties arise on relevant experimental studies.However，a noticeable unbalance between the rates kdand βeito trigger the electron detachment instability mechanism treated can easily be realized in large gas volumes too.In this respect，a very efficiency is the heating of SF6-based gas mixtures by a pulsed CO2laser radiation.It is this method that we have used in the present paper to study the SSVD instability caused by electron detachment from negative ions by electron impact in SF6and SF6-based mixtures，including working media of HF（DF）lasers.

2 Experimental

The experimental set-up（see Fig.1）and measuring technique did not differ appreciably from those used by us previously in Ref.[11］.An SSVD was investigated in SF6and mixtures of SF6with C2H6，H2， and Ne at a partial SF6pressure pSF6=2.0 kPa and the total mixture pressures of up to 6.6 kPa.The discharge was triggered in the needle（cathode）-cylinder（anode）geometry at an interelectrode distance of 43 and 53 mm.The needle was simulated by a copper rod segment dressed with a polyethylene jacket.The cathode was armored in a segment of a 15 mm inner diameter dielectric tube extending by 12 mm above the needle tip.The specific electric energy depositions Welwere varied in the range from 0.02 to 0.2 J/cm3.

Fig.1 Experimental setup.

A preliminary gas heating was performed only within a narrow zone of the discharge gap on illumination，the gap by a pulsed CO2laser through a 10 mm slit diaphragm arranged normal to the electric field direction（see Fig.1）.As will be inferred from the following，this irradiation scheme allows observing the SSVD constriction immediately in the bulk of the heated gas（like that in a glow discharge[12，14］） rather than in the form of a single channel growing from the cathode spot and bridging finally the discharge gap[15］.The gas temperature Tgestablished in the SSVD burning region was determined both by the laser radiation energy absorbed by SF6molecules[13］and by the propagation velocity of the shock waves formed at the boundaries between the heated and cold gas[16］.The temperature Tgchanged from 800 to 2 100 K（the specific energy Waof the laser radiation absorbed by SF6in the SSVD burning region was 0.05-0.23 J/cm3）.The voltage pulse was applied with a delay of 4 μs relative to a 3 μs laser pulse at level of 0.1（the delay was kept from the leading edges of the pulses[17］），which ensured the establishment of the thermal equilibrium between the translation and internal degrees of freedom of the irradiated gas components by the instant of triggering the discharge in the pressure range studied[18］.

In the experiment，monitoring of the SSVD voltage and current was performed with a resistive voltage divider and low-resistivity shunt，respectively.The SSVD was also filming using a digital camera synchronized with a laser pulse.To identify basic processesdetermining the SSVD voltage-current characteristics，we also recorded the voltage and current oscillograms of a confined discharge，which allowed us to eliminate the influence on the discharge voltage and current of the factors coming from extending the discharge volume on increase in the energy input into the plasma[19］.To this end，the SSVD was triggered in a quartz tube of 8.5 mm in diameter at the interelectrode distance of 43 mm（the needle-plane geometry）.Experimental oscillograms were compared with the calculated ones（the design procedure is described in Ref.[20］）.

3 Experimental results

In Fig.2（a）and 2（b）are given the SSVD photographs in mixture SF6∶Ne∶C2H6taken at Wel=0.15 J/cm3，discharge current duration τdis=270 ns and different Tgvalues.

Fig.2 Photographs SSVD at Tg=1250 K（a）Tg=900 K（b）；distributions of SSVD radiation intensity F along the coordinate X in Tg=1 250 K（c）and Tg=900 K（d）.Mixture SF6∶Ne∶C2H6=5∶5∶1，p=4.4 kPa，Wel=0.15 J/cm3，τdis=270 ns.

Fig.2（c）and（d）show the corresponding discharge plasma glow intensity distributions along the X-axis passing through the middle of the heating zone in parallel to its boundaries（see Fig.1）.In the heating region，the SSVD is seen to show a filamentary-like spatial plasma（current）structure close to a quasi-periodical structure.A spatial period of the formed structure decreases on increasing Tgvalues. Despite a filamentary-like SSVD structure，plasma channels in the heating zone possess a diffuse character at moderate values of Weland τdis.Increase in Welor τdisresults in the dominance of a single channel（as a rule，in line with the central electric field tube）and its constriction.It is significant that similarly to cold gas[19］the SSVD constriction threshold in pure SF6is lower than in SF6-C2H6mixtures with respect to parameters Weland τdis.By way of example，F(xiàn)ig.3（a）and（b）shows the SSVD photographs in mixture SF6∶Ne∶C2H6（Fig.3（a））and pure SF6（Fig.3（b））taken at（a）τ=270 ns and Wel=0.2 J/cm3； （b）τ=150 ns and Wel= 0.11 J/cm3.It is seen that the instability develops immediately in the irradiated region of the discharge gap.Some analogy appears to be appropriate here with the low-pressure glow discharge constriction[12，14］.On further increase in Welor τdis，a spark channel bridges the whole gap.At constant values of Weland τdisthe SSVD constriction probability may also increase with increasing Tgin the irradiated zone of the gap.

Fig.3 Photograph of SSVD in mixture C2H6∶SF6∶Ne= 1∶5∶5，Wel=0.2 J/cm3，Tg=1 250 K，τdis= 270 ns and p=4.4 kPa（a）；pure SF6，Tg= 1 100，τdis=150 ns，Wel=0.11 J/cm3and p= 2.0 kPa（b）.

The voltage oscillogram of a confined SSVD in SF6taken at p=2.0 kPa and Wel=0.12 J/cm3has been compared with the relevant voltage time dependences calculated accounting for the following processes：electron impact ionization and attachment；ion-ion recombination with the rate constant βei=2×10-8cm-3[21］；dissociative electron-ion recombination（the corresponding rate constant was varied within the range 0.5-3×10-7cm-3）；electron detachment of electrons from negative ions by electron impact，kd=3×10-7cm-3[22］；SF6dissociation by electron impact，the energy for F-atom formation was～4-6 eV，according to different data（see Ref.[23］，[24］and references cited therein）.The best agreement between the calculated time dependences and the experimental oscillogram，as mentioned，has been attained at βei≈kd.

Given all the above，the following three key features should be kept in mind on analyzing the SSVD instability mechanisms in SF6-based mixtures，including working media of HF lasers：

First，an SSVD in the heating zone shows a filamentary quasi-periodic structure，with the spatial period depending on Tgvalue；

Secondly，the instability development of an SSVD starts from its constriction immediately in the irradiated zone of the discharge gap；

Thirdly，at room temperatures，electron multiplication due to electron detachment from negative ions by electron impact is compensated for electron losses in the process of electron-ion recombination（βei≈kd）.

4 Discussion

4.1 Nonlinear mechanism of ionization multiplication in working media of HF（DF）lasers

In SF6at room temperature T0and（），the rate constant for the electron impact formation ofis approximately twice as large as that forproduction[26］.In a laser-heated gas，the situation may be different.Indeed，the reduced electric field becomes appreciably higher compared to（，because of electron attachment to vibrationally excited molecules of SF6[16，27］.Considering the electron impact rate at higher gas temperatures to be not less than that at room temperature，we can assume that the total electron attachment rate increases too. However，whether vibrational excitement affects the relative yield of negative ionsandand in which way is not clear at present.Therefore both the negative components mentioned are to be dealt with.

The electron detachment from negative ionsby electron impact was first considered in Ref. [22］.There have been some quantitative assessments in Ref.[22］，which give convincing evidence of this process to be very efficient.The corresponding rate constant was estimated to equal kd（）= 3×10-7cm3/s.This assessment proceeded from the assumption that the cross-section for the electron detachment by electron impact is not less than that of the electron elastic scattering，which is in excess of 10-15cm2[25］. Account was also taken of the electron affinity to SF6molecules（0.65-1 eV[25］） to be much less than the mean electron energy〈ε〉～8-10 eV at the reduced electric fields approaching the critical one[25］.Therefore the electron detachment fromby electron impact may be thought of as a non-threshold process.As forhaving the electron affinity Eaff～2.8 eV[25］，the corresponding electron detachment rate should be reduced compared to that of the elastic scattering by approximately 40％ accounting for the Boltzmann factor exp（-Eaff/T*），T*＜2〈ε〉/3.Therefore，the difference betweenandcan actually be neglected and，correspondingly，some averaged detachment constant kdbe taken.

Keeping the aforesaid in mind and aiming mainly at a qualitative insight into the nature of the instability induced by electron impact detachment，we may give the relevant system of equations in the form

Here neand Nnare the electron and negative ion densities，respectively；α and η are the electron impact ionization and electron attachment coefficients，ueis the electron drift velocity.It should specially be stressed that in strongly electronegative gases，like those treated in this study，the ion densities may be much larger than the electron ones. Therefore the electron losses due to electron-ion recombination in these gases take on much greater importance as compared to that in electropositive ones. This particular feature permits us also to ignore termin equation（1）.In addition，no account is taken of the ion-ion recombination process in equations（1）and（2）.Because of a fairly low recombination rate constant βiiat the reduced electric fields approaching（E/N）cr[21］，this process comes into play only at a final stage of SSVD and does not appear to affect radically a general pattern of the instability growth described by equations（1）and（2）.

Equations（1）and（2）may be reduced to a single nonlinear integro-differential equation describing the electron multiplication in active media of HF（DF）lasers[11］.In Ref.[11］，exact analytical solutions for ne（t）have been obtained.They radically depend on parameter ξ[11］：

where ne（0）is the electron density at the initial stage of the quasi-stationary phase.

Let there be ξ＞0.Then

At sufficiently low ne（0）values and/or closely spaced rate constants kdand βei，the electron density does not increase noticeably by the instant the discharge current reaches its maximum.The first is realized at small enough specific electric energy depositions Welwhatever should be kdand βei.In this case λ→0 and the solution（4）goes into an ordinary electron multiplication law

as if the electron detachment from negative ions by electron impact were absent.That is typical of an SSVD in SF6-based mixtures at Welvalues being less 50 J/L even in the laser-heated regions.The second possibility（kd≈βei）is characteristic of the shockcompressed gas regions sandwiched between the shock wave fronts and the contact discontinuity surfaces wherein the gas temperature is nearly that of the undisturbed regions.

At ξ＜0，the electron detachment from negative ions plays the predominant role and the expression obtained for the electron concentration

does not go into（3）whatever be ne（0）and kdβei.

It follows from expressions（3），（4）and（6） that at unbalance between the detachment and recombination rates（kd-βei＜0）at the stage of increasing the discharge current（α＞η）both solutions（4）and（6）manifest a pronounced“explosive”character，i.e.some finite time after the ionization process starts the electron concentration becomes arbitrary large.Expressions（4）and（6）allow the characteristic＂explosion＂timesto be easily determined.

If ξ＞0，then

At ξ＜0

In reality，of course，the result obtained means that in a lapse of a certain timethe electron attachment is partly compensated for by their detachment from negative ions by electron impact.By analogy with the terminology used in the theory of excimer lasers，this process may be called the“burning away”of electronegativity，because in this case we deal with not destruction of electronegative molecules but with losing the ability to capture free electrons because of the electron detachment process.

At the stage of decreasing，the discharge current in the SSVD quasi-stationary phase α＜η，and，correspondingly，a＜0.It follows from relationships（4）and（6）that in this case the electron concentration always tends to zero with time.In other words，the volume electron multiplication due to electron detachment from negative ions by electron impact is not capable of being competitive with the attachment-induced electron losses if the electron capture by molecules is more efficient than impact ionization.As a result，in the SSVD quasi-stationary phase ionization instability arising from the“explosive”character of electron multiplication can develop only at the stage of current increase.

4.2 Self-organization of the SSVD plasma on laser heating of SF6-based mixtures

The nature of self-organization of the SSVD plasma in heated SF6-based mixtures is not quite clear.In our opinion，this phenomenon can substantially be connected with the development in the SSVD plasma of the ionization instability caused by the electron detachment from negative ions（see above）. We now advance some relevant qualitative arguments.

At high gas temperatures kd-βei＞0，which results in an“explosive”growth of ne（t）on increasing the discharge current（α＞η）.The current passage through the discharge gap in the SSVD quasistationary phase is controlled by LC-circuit with a characteristic time τc～， which is several hundreds of nanoseconds under the conditions of interest，whereas～20-30 ns.Since，it must necessarily result in the SSVD quasi-stationary phase（E/N≈（E/N）cr）in the current redistribution over the discharge gap to form separate longitudinal current layers（thin filaments at high Tg-values）with an enhanced electron concentration. Indeed， a standard linear analysis shows that it is normal to the current direction spatial perturbations that possess the largest increments of growth.In the nonlinear stage of the perturbation development，there can be formed the quasi-periodic structures observed in the experiment.

Following the Ref.[28］，it is easy to show that the structures in the form of separate filaments are stabile.On rising the gas temperature，the difference kd-βeialso increases，which results in a more rapid growth of ne（t）.One can therefore assume that it is for this reason that the number of conducting channels increases with growing Tgand，hence，the spatial period of the current structure decreases. An additional argument in favor of the above considerations is also the fact that at extremely low Tgvalues realized in the experiment the quasi-periodic structures did not appear at all.Indeed，in this case

At the stage of decreasing the discharge current the above-considered“explosive”mechanism is not possible because E/N＜（E/N）crand α＜η（see section 4.1）.In this case the instability development can develop at a falling section of the quasistatic U-I characteristic（the relaxation U-I characteristic time τUI?τc）controlled by the effective ionization coefficient αeff（ne）=α-η+（kd-βei）nn（ne）/ue.In doing so，the excess of the attachment rate over that of impact ionization is compensated for electron detachment of electrons from negative ions by electron impact.The SSVD on this portion of the U-I characteristic is unstable with respect to spatially homogeneous fluctuations of the plasma parameters. However，spatially inhomogeneous fluctuations can develop in the SSVD plasma followed by formation of spatial structures comprised of separate current filaments with an enhanced electron density.The relevant scenarios of such a self-organization and the problem of the formed plasma structures stability have been considered in greater detail in the literature（see Ref.[28，29］）.Besides，there are certain grounds to believe that the SSVD constriction at long duration discharge pulses does occur at the falling section of the U-I characteristic，too.

4.3 On the mechanism of propagation of conducting channels in SF6and its mixtures

A nonlinear electron multiplication mechanism due to unbalance between the rates of electron detachment by electron impact and electron-ion recombination can also affect the propagation of conducting channels in SF6-based mixtures through the discharge gap at room temperatures if，as already mentioned，E/N（E/N）cr.Such is the case in the vicin-ity of a single conducting channel growing from the cathode side.

The reduced electric field at the tip of this channel exceeds appreciably（E/N）cr[15］.It leads to a significant increase in Tevalue and，consequently，to noticeably decreasing βei（see Introduction）.A situation arises，when again，as at high gas temperatures，the difference k0-βei＞0.It triggers the above considered mechanism of an“explosive”electron multiplication，thereby forms a new plasmafilled segment of the channel ensuring the channel advancement into the interior of the discharge gap. Therefore there are no grounds to invoke a stepwise mechanism of ionizing SF6molecules，suggested in the Ref.[10］，in order to explain the propagation of conduction channels in SF6and its mixtures.

5 Conclusions

In the present paper，a fundamentally novel mechanism of the detachment instability developed in active media of HF（DF）lasers due to electron detachment from negative ionsandby electron impact is investigated.Based on principal mechanisms of formation and destruction of negative ions in SF6and its mixtures，it is shown that the instability arises from the unbalance of the rate constants for electron detachment from negative ions by electron impact and dissociative electron-ion recombination. Analytical expressions for increasing the electron concentration in time are obtained.It is shown that on increasing the discharge current，the instability development displays an“explosive”character；the characteristic“explosion”time is assessed.On laser heating SF6-based gas mixtures by a pulsed CO2laser radiation，the development of the instability studied has been initiated in large gas volumes with the aim of its experimental study.A plausible connection of this process with a spatial self-organization（formation of current filaments）in the SSVD plasmas of the pre-irradiated SF6and SF6-based mixtures is discussed.The mechanism of propagation of an incomplete channel owing to electron detachment from negative ions by electron impact has been considered.

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Author′s biography：Sergey Kazantsev（1971—），Moscow，Russia，graduated from Moscow Engineering Physics Institute（State University）in 1998，His research interests are concerned with experimental investigation of volume selfsustained gas discharge phenomena，development of chemical and high-power electric discharge lasers，and investigation of high power laser beam interaction with matter，laser induced gas breakdown，laser lightning protection.E-mail：kazan@kapella.gpi.ru

非鏈式化學HF（DF）激光器工作氣體中電子分離的非穩(wěn)定性和氣體放電等離子體的自組織現(xiàn)象

BELEVTSEV A A1，F(xiàn)IRSOV K N2，KAZANTSEV S Yu2，KONONOV I G2，張來明3

（1.俄羅斯科學院高能密度研究所高溫實驗室，莫斯科125412；2.俄羅斯科學院普羅霍羅夫普通物理研究所，莫斯科119991；3.中國科學院長春光學精密機械與物理研究所，激光與物質(zhì)相互作用國家重點實驗室，吉林長春130033）

1674-2915（2011）01-0031-10

2010-08-13；

2010-10-15

Supported by Russian Foundation for Basic Research Project（Grants No.08-08-00242 and 09-02-00475）.

報道了放電引發(fā)的非鏈式HF（DF）激光器中的激活介質(zhì)由電子碰撞負離子分離引起的電離非穩(wěn)定性。這種非穩(wěn)性出現(xiàn)在電極空間分離、脈沖CO2激光加熱的基于SF6的混合氣體的大體積放電中。實驗研究了自引發(fā)體放電過程中由激光加熱引起的放電等離子體的自組織現(xiàn)象以及由此在放電間隙的大部分區(qū)域形成的準周期等離子體結(jié)構(gòu)。重點分析了等離子體結(jié)構(gòu)隨氣體溫度和注入能量的變化，討論了等離子體自組織對電子碰撞分離不穩(wěn)定性所產(chǎn)生的影響，解釋了混合氣體中由于電子碰撞使負離子消失導致的單等離子體通道移動的產(chǎn)生機理。

HF/DF激光器；電離非穩(wěn)定性；自組織現(xiàn)象；自引發(fā)體放電；等離子體結(jié)構(gòu)

TN248.5

A

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