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28th ICPIG, July 15-20, 2007, Prague, Czech RepubliF Topic number: 15 Low pressure (rare gas + water vapor)-discharge as a light source: (2) electrical characteristics E. Artamonova1, T. Artamonova1, A. Beliaeva1, D. Gorbov1, D.Michael2, M. Khodorkovskii1, A. Melnikov1, V. Milenin1, S. Murashov1, L. Rakcheeva1, N. Timofeev1, G. Zissis3 1 Saint-Petersburg State University, Ulyanovskaya 3, 198504, Russia 2 General Electric Global Research Center, Niskayuna, USA 3 Paul Sabatier University, Toulouse, France The strength of the electric field, electrode fall voltage, light emission and light efficiency of an (Ar + H2O) DC discharge as functions of water vapor content, argon pressure and electric current are presented. Obtained data make it possible to conclude that the light efficiency of the plasma under study can reach 30-40 Lum/Wt. 1. Introduction The first part of the study [1] devoted to the investigation of spectroscopic and energetic characteristics of a low pressure low current discharge in the mixture of a rare gas (Ne, Ar, Kr or Xe) and water vapor showed that the (Ar + H2O)discharge, in comparison with the discharges with the other rare gases, has some prospects as a light source. It was shown that under studied discharge conditions the light efficiency of the discharge in question reached (20-22)% of a mercury fluorescent lamp efficiency, the lifetime of an (Ar + H2O)-lamp being several weeks. The UV radiation exciting a phosphor and defining discharge lighting properties was OH 306.4 nm. Unfortunately, the way (ways) of the water molecule destruction and the hydroxyl molecule excitation in the plasma in question are not clear wholly. The present paper is the continuation of [1] and describes the data of probes measurements of the strength of the electric field in the positive column of an (Ar + H2O)-discharge, electrodes fall voltage and the dependencies of some electric, spectroscopic and energetic characteristics on the discharge parameters. In addition to the new information about the discharge these data could also make it possible to estimate light efficiency of a positive column and make more clear the picture of plasma-chemical processes taking place in the (Ar + H2O)-plasma. The latter is very important due to the fact that the further progress is surely connected with the elucidation of these processes. discharge two molybdenum cylindrical probes are inserted into a tube. Probes are 0.2 mm in diameter and 1.5 mm in length. The probes are placed in the axis of the tube perpendicular to its axis. The scheme of the E-measurement is shown in Fig.1. The every probe is connected to the “ground” potential with the help of two resistances, one of them having the large value 5.4 MΩ, so that the probe potentials are almost the floating ones. Two signals, proportional to the probe floating potentials, come to the input of a differential amplifier. The output signal of this amplifier is the subtraction of input signals. It comes to the millivoltmeter and to the analog-digital converter (PUPSIK), and then to a computer. The floating potential does not coincide with the plasma potential, so such measurements give the strength of the electric field E in the positive column and make it possible also to derive the total electrodes fall voltage Uelectrode, i.e. the sum of cathode and anode fall voltages. 2. Experimental In general the experimental equipment and the procedure of (Ar + H2O)-mixture preparation and further discharge operation is similar to that of described in [1]. For the measurement of the strength of the electric field E in the positive column of the Fig.1. The scheme of the set-up for the measurement of the strength of the electric field E. 3. Results Discharge characteristics – the strength of the electric field E in the positive column, electrodes fall 1213 28th ICPIG, July 15-20, 2007, Prague, Czech RepubliF voltage Uelectrodes, phosphor emission I and light efficiency I/W of a discharge (W is the discharge consumed electric power) – have been measured in dependence on the argon pressure in the range (0.520) Torr, value of the electric current in the range (0.1-0.6) A, and quantity of water molecules added to the discharge volume. The water vapor pressure is defined by the tube wall temperature and is in the range (0-80) mTorr. The strength of the electric field as a function of the argon pressure and the tube wall temperature is shown in Fig.2. At 20C, when the effect of water molecules is negligible, E is in a good agreement with the known data (see e.g. [2, 3]). products begin to define plasma properties. At the lowest investigated argon pressure the rise of PAr from 0.5 Torr till 1.0 Torr leads approximately to twice diminishing of E at all studied T. It is possibly connected with the fact that, in spite of the essential increase of water molecule concentration, argon atoms mainly define the ionization processes in the plasma as before. The rise of E as a function of T is different at different argon pressure and is considerable: from ~ (1-2) V/cm at 20C till ~ (1326) V/cm at (70-80) C. The electrodes fall voltage Uelectrodes dependences on the argon pressure and on the tube wall temperature shown in Figs.3 are in general similar to that of the E dependencies. 20C 30C 40C 50C 60C 70C 30 25 20C 30C 40C 50C 60C 70C 110 100 90 20 15 Uelectrodes, V E, V/cm 80 10 70 60 50 40 5 30 20 0 0 5 10 15 20 0 PAr, Torr 5 10 a) 30 26 24 22 Ar0.5Torr Ar1.0Torr Ar3.5Torr Ar10Torr Ar20Torr 110 100 90 20 18 80 16 70 14 Uelectrodes, V E, V/cm 20 a) 0.5 Torr 1.0 Torr 3.5 Torr 10 Torr 20 Torr 28 15 PAr, Torr 12 10 8 6 60 50 40 4 30 2 0 20 20 30 40 50 60 70 80 10 t, C 20 30 40 50 60 70 80 T, C b) Fig.2. The strength of the electric field E as a function of argon pressure (a) and the tube wall temperature T (b) i = 0.3 A. Addition of water vapor makes the curve E(PAr) as a whole to move up, the bigger the tube wall temperature the higher the curve position. The tendency of E to be weakly changed for PAr > 10 Torr means that water molecules or their dissociative b) Fig.3. The electrodes fall voltage Uelectrodes as a function of argon pressure (a) and the tube wall temperature T (b). PAr. i = 0.3 A. However its rise is considerably less – in (2-4) times, while E changes approximately in an order at corresponding changes of the discharge conditions. Most likely, similarly to a mercury fluorescent lamp 1214 28th ICPIG, July 15-20, 2007, Prague, Czech RepubliF discharge as a whole. The light efficiency of the discharge as a whole is ~ (20-22) Lum/Wt, so the reachable value of the efficiency is (30-40) Lum/Wt. Relative to the mercury fluorescent lamp efficiency this gives 0.06-0.09 that is very close to the estimation made in [1]. Fig.5 shows E as a function of i at different tube wall temperature. The dependency is as expected: E falls with the increase of the electric current i. The similar dependence has been obtained in the whole argon pressure diapason investigated in the work. One could notice that at the low water content (at the low tube wall temperature) the relative decrease of E with the increase of the electric current value i is more noticeable than at the higher tube wall temperatures. Most likely, the reason is connected with the Maxwellization of the electron energy distribution function and increasing role of collisions with water molecules when T rises. o 12 11 10 9 8 7 6 5 T8 with probes. Ar. i=300 mA. Wac/Wcol T=10 C o T=20 C o T=30 C o T=40 C o T=50 C o T=60 C o T=70 C 13 E, V/cm [4], it is explained by prevailing of argon atoms ionization over the ionization of additive atoms (mercury) or molecules (water, hydroxyl) nearby electrodes. Moreover the identity of E(PAr, T) and Uelectrodes(PAr, T) proves that the main ionization mechanism in the plasma in question is also the ionization of argon atoms. Note that in spite of the common opinion (see e.g. [4, 5]) water vapor does not influence crucially on the operation of oxide electrodes. It is true both for the value of the electrodes fall voltage and the tube lifetime. Fig.4 presents the ratio of the power Wac consumed by a discharge as a whole to the power Wcol consumed by a positive column in dependence on the total discharge voltage Uac. The discharge voltage rises with the rise of the tube wall temperature and, as an experiment shows, is a very good indicator of the water vapor influence on the discharge characteristics. Wcol is obtained in the assumption that the length of the cathode and anode regions is much less than the length of a positive column. The general tendency of the obtained behavior of this ratio is falling with the discharge voltage rise. It is explained by sufficiently bigger rise of the electric field strength in comparison with the rise of the electrodes fall voltage when the tube wall temperature is increasing. 4 3 2,6 2,5 2,4 2,3 2,2 2,1 2,0 1,9 1,8 1,7 1,6 1,5 1,4 1,3 1,2 1,1 2 Wac/Wcol 0,5 torr Ar 1 torr Ar 3,5 torr Ar 10 torr Ar 20 torr Ar 1 100 200 300 400 500 600 i, mA Fig,5. The strength of the electric field E as a function of the electric current i at the different tube wall temperature. The argon pressure is 1 Torr. o 0 50 100 150 200 250 300 350 400 450 T=10 C o T=20 C o T=30 C o T=40 C o T=50 C o T=60 C o T=70 C 34 Uac, V 32 Fig.4. The ratio of the discharge consumed electric power Wac/Wcol to the electric power dissipated in the discharge positive column in dependence on the discharge voltage at different argon pressure. i = 300 mA. 28 Uelectrode, V These data make it possible to define the efficiency of the positive column in the mixture of argon and water vapor and estimate the maximum efficiency that can be reached with lengthening a discharge tube. The highest discharge light efficiency for the tube configuration in question is obtained when the water vapor pressure is so that the total discharge voltage is about (60-80)V. At this discharge voltage the efficiency of the positive column is ~ (1.5-1.8) times higher then that of the 30 26 24 22 20 18 100 200 300 400 500 600 i, mA Fig.6. The electrodes fall voltage Uelectrodes as a function of the electric current i at the different tube wall temperature. The argon pressure is 1 Torr. 1215 28th ICPIG, July 15-20, 2007, Prague, Czech RepubliF The electrodes fall voltage Uelectrodes as a function of the electric current i is shown in Fig.6. It also changes rather weak with the increase of the electric current, so that in the first assumption one can consider Uelectrodes as independent on i. Similar data have been obtained for the whole investigated diapason of argon pressure. The phosphor emission caused by the UV radiation of the discharge positive column is shown in Fig.7. At the low tube wall temperature the role of water molecules is negligible, and the light emission of a phosphor is low and even slightly decreases with the rise of the electric current. Addition of water molecules into the discharge leads to the appearance of OH 306.4 nm band radiation which excites a phosphor. The light emission increases and its current dependence becomes rising and close to linear at T > 40C. Usually the rise of i causes the proportional rise of the electron density, so one can conclude that the phosphor emission becomes proportional to the electron density o T=1,2 C o T=5 C o T=20 C o T=30 C o T=40 C o T=50 C o T=60 C o T=70 C 250 I, rel. un. 200 150 100 50 0 100 200 300 400 500 600 i, mA Fig.7. Light emission of (Ar + H2O)-discharge as a function of the electric current i. PAr = 6 Torr. The light efficiency at T ≤ 20C falls down with the increase of the electric current due to the rise of the consumed electric power and merely constant light emission (see Fig.7). Addition of water vapor leads to the rise of the light phosphor emission that makes the efficiency merely independent on the electric current at T ≥ 40C. 4. Discussion In addition to the study of some electric discharge characteristics the important task of the study is to inquire the processes that could be responsible for the excitation of hydroxyl molecules. In this aspect the current dependencies of plasma characteristics can be fruitful to make some conclusions about the question. Analysis of the balance equations for the main participants of the plasma processes (argon metastable atoms, water molecules, hydroxyl molecules in the ground and excited states, hydrogen atoms) that take into account the main processes with their participation (quenching of excited argon atoms by electrons and water molecules, diffusive losses of hydroxyl molecules and hydrogen atoms that, as simple estimations show, are their main disappearance processes in the plasma in question, and radiative destruction of excited hydroxyl molecules) shows that the linear increase of the phosphor emission at the water vapor presence in the plasma can be explained only by two processes: 1) quenching of an argon excited (metastable) atom by a water molecule and 2) dissociation of a water molecule by an electron collision with simultaneous excitation of OH. The latter is less probable [1], so the role of argon metastable atoms in the plasma is defining. The solution of the balance equations shows that when the role of water molecules in quenching of argon metastable atoms is sufficiently weaker than that of the electron one, the concentration of argon metastable atoms does not depend on the electron concentration. This is in a good agreement with the experimental data [2, 3] and the data of Fig.7 where the weak current dependence of I at the low tube wall temperature is noticeable. When, oppositely, the water molecule destruction of argon metastable atoms prevails the electron one, the concentrations of hydroxyl molecules in the ground and excited states and the concentration of atomic hydrogen become independent on the water molecule one. The phosphor emission I of the discharge is caused by the hydroxyl radiation 306.4 nm and hence in this case the phosphor emission is independent on the water concentration, i.e. on the tube wall temperature T. Fig.3a [1] confirms this conclusion – the phosphor emission changes negligible at T ≥ 60C. The study is partly supported by RFBR, grant No 06-02-17326a. 5. References [1] E. Artamonova et al, Proc. 28th ICPIG. [2] V. Granovsky, Electric current in a gas. Steady-state current, “Nauka” Publ., Moscow (1971). [3] Yu. Kagan, R. Liagustchenko, A. Khakhaev, Optika i spectroskopia 14 (1963) 538; 15 (1963) 13. [4] G. Rokhlin. Discharge light sources, Energoatomizdat, Moscow (1991). [5] J. F. Waymouth. Electric discharge lamps, The M. I. T. Pres, Cambridge, Massachusetts and London, England (1971). 1216