CP620, Shock Compression of Condensed Matter - 2001 edited by M. D. Furnish, N. N. Thadhani, and Y. Horie © 2002 American Institute of Physics 0-7354-0068-7/02/$ 19.00 NICKEL CRITICAL POINT PARAMETERS FROM SHOCK EXPERIMENTS WITH POROUS SAMPLES Dmitry N.Nikolaev, Vladimir Ya.Ternovoi, and Alexei A.Pyalling Institute of Problems of Chemical Physics RAS, Chernogolovka, Russia, 142432 Abstract. Results of experiments on expansion of shock-compressed nickel samples into helium is presented. The brightness temperature of nickel sample and shock velocity in helium were measured by an optical pyrometer, other parameters (particle velocity, pressure, helium temperature) were calculated. To increase the shock entropy up to near-critical value, shock compression of porous (m=1.91) samples were used. Isoentrope with initial pressure 170 GPa was studied, with final states below 1.4 GPa, determined by initial helium pressures. The peculiarities of isentrope slope in pressure-particle velocity graph allowed to estimate a point of it's entrance into two-phase region. The isobaric overheat of expanded nickel by hot shocked helium allowed to get an additional information about phase diagram and to estimate of critical temperature and pressure of nickel, using the van-der-Waals model of liquid nickel spinodal. Registration of light emission snapshot of unloading specimen gives us the velocity of shock in helium, and, using helium EOS, we can calculate particle velocity and final pressure of expanded metal. Because of it's relative high ionization potential, helium remains transparent in shocked state, that makes possible to register emission from metal surface and to calculate it's brightness temperature. So the isoentrope can be traced on both pressure - particle velocity and pressure - temperature planes. The results [1-4] were obtained for Pb and Sn metals with quite low values of critical entropies, that allows to investigate near-critical and even supercritical isoentropes, using existing explosive launchers with well-defined performance. Investigation of metals with high critical parameters requires strikers, accelerated to velocities more than 10 km/s. Elaboration of such launchers is serious technical problem, not solved INTRODUCTION The method of shock loading and isoentropic expansion of matter allows one to exceed limitations of both static methods and common Hugoniot measurements, and provides the opportunity to investigate thermodynamics of liquid - vapor phase transition in near-critical point region. In particular, this method was used to investigate location of coexistence curve and critical point in the P-T phase diagram of lead and tin [1-4]. In this experiments release isoentropes were traced for several initial Hugoniot pressures. A number of final pressures on isoentrope was defined by variation of shock compressibility of obstacle medium. Helium was used as obstacle, and variation of its initial pressure from zero to more than 100 bar was enough to trace isoentropes in wide range of parameters. 59 20000 T,K 15000 10000 5000 f 0 200 FIGURE 1. Experimental assembly. 1 - diaphragmed optical fiber, 2 — pressurized case, 3 — glass window, 4 — helium under pressure, 5 - porous nickel sample, 6 — steel bottom of assembly, 7 — steel striker 400 600 800 t, ns 1000 FIGURE 2. Typical experimental snapshot. Emission intensity already recalculated in brightness temperature. up to now. For achieving the required near-critical entropy with common launching systems, the use of porous specimen was proposed. It also solves another problem: if striker velocity will be very high, the temperature of shock-compressed helium would be sufficient to it's noticeable ionization and, thus, loss of transparency. In this situation pyrometer would register the emission of shocked helium. photoreceivers at several wavelengths. To transmit emission from assembly, quartz-polymer optical fiber with diaphragm on assembly end was used. Light was collected from little area of 2-3 mm diameter. Before each experiment, pyrometer, connected with fiber and diaphragm, was calibrated, using standard tungsten ribbon lamp, so brightness temperatures on various wavelengths can be calculated. Typical experimental snapshot is presented on Fig.2. For calculating of shock velocity in helium we needed a precise value of distance between window and nickel surface. At high initial pressures of helium the bottom bulge can add sufficient error in distance measurement, so the dependence of bulge from initial pressure in assembly was measured. Parameters of shock wave in helium were calculated using plasma EOS [5], although discrepancy between EOS data and basic expression for monoatomic ideal gas (D = 4/3Up) wasn't higher than few percents. EXPERIMENTAL TECHNIQUE Experimental assembly, used in experiments with porous nickel samples, was analogous to that, used in experiments with lead and tin [4]. Porous samples, 20mm diameter, were compacted from nickel powder in hydraulic press. Thickness of the samples was chosen about 0.2 - 0.3 mm, to avoid an overtaking of shock wave by release wave. Samples with mean density m = p/po = 1.91 (p sample density, p0 - normal density of nickel) is quite firm, and, glueg to bottom, can follow the bottom bulge under helium pressure. Experimental is shown on Fig.l. The sample was loaded by impact of steel striker, accelerated by 2-stage explosive launching system. Hugoniot pressure in samples was 1.7 GPa. Thermal emission from assembly was traced by fast multichannel pyrometer with p-i-n photodiodes as RESULTS AND DISCUSSION Experimental results obtained is presented on Fig.3 and 4 and in Table 1. As was shown in [6], a sharp change in slope of isoentrope on pressure particle velocity plane caused by formation of shock boiling wave in the moment of it's entrance 60 in two-phase region. Thus we can assume, that this isoentrope crosses with saturation curve at 0.080.09 Gpa. The process of shock exit on the surface of sample would be accompanied by various instabilities, led to intense mixing of Ni and He and heat-mass exchange. Actually, in experiments with compact samples we registered the process of overheating of sample surface by hot shocked helium and used this data to trace liquid spinodal of metals. In case of porous Ni the process of heat-mass 0.20 0.00 4000 6000 8000 10000 12000 14000 16000 T,K EOS spinodal —— Van-der-Waals spinodal + Cp, Bushman, Lomonosov D Cp, our estimation EOS Isoentrope Cp, Young, 1971 Cp, Fortov, Yakubov, 1994 Ni temperature He temperature FIGURE 4. P-T graph. Experimental points - temperature of helium and temperatures of Ni overheat. lead and tin the temperature anomaly was fond. At pressures, close to critical, process of heat-mass exchange becomes supereffective, and temperatures of overheat of metal surface raised close to helium temperature. On nickel P-T diagram (Fig.4) one can see this anomaly at pressure about 0.9 GPa. We suppose, that this is a critical pressure. This value don't contradicts with existing theoretical predictions. For estimation of critical temperature, van-derWaals model of liquid spinodal was applied. If we know critical pressure and have measured an experimental spinodal points, it's possible to construct liquid spinodal, and find a critical temperature. In our case Tcr.p. = 9100 K. It should be pointed, that van-der-Waals model is the most simple model of phase diagram. A lot of other models exists, and we can use it for this calculations, for example, spinodal [9]. Another anomaly on experimental spinodal exist at pressure of isoentrope entrance in two-phase region. As mentioned above, this is connected with formation of shock boiling wave. Now we can estimate parameters of critical point of nickel. IE-3 FIGURE 3. P-Up graph. Curves - EOS [7] calculation of release isoentropes with various initial porosity of sample. transfer become so fast, that it's impossible to register the initial temperature of metal surface, moreover, in some experiments we obtained a slow cooling of initially hot surface. So we accepted, that in experiments with porous samples measurements of temperature on isoentrope is impossible, and only the temperature of overheat (spinodal temperature) can be measured. Our experience confirms, that this information is significant for understanding of phase diagram. If investigated isoentrope passes considerably near critical point, it can get into region of low mechanic and thermodynamic stability [8], where anomalies in compressibility, heat conductance and sound speed is predicted. In P-T graphs of both 61 TABLE 1. Experimental data on isoentropic expansion of Ni. Initial Hugoniot pressure l.TGPa. Po, Bar D, km/s Up, km/s P,GPa THe,K T,K M AUp, km/s AT, K 0.056 0.51 0.85 2.005 3.46 10.1 11.6 13.557 22.19 25.33 27.24 34.9 39.14 48.09 30.2 48.09 66.14 67.7 60.02 58.76 67.71 87.33 101.6 117.5 16.96 14.56 14.46 13.25 11.79 11.77 11.16 12 11.26 11.2 11 11.05 11.13 10.84 11.08 11.49 9.86 9.95 10.61 11.04 10.85 9.76 9.91 9.8 13.78 11.12 10.99 9.92 8.78 8.76 8.3 8.94 8.38 8.36 8.17 8.22 8.28 8.07 8.24 8.56 7.31 7.38 7.89 8.21 8.07 7.22 7.31 7.21 0.002185 0.0138 0.0226 0.0441 0.0715 0.174 0.18 0.244 0.351 0.396 0.41 0.531 0.605 0.705 0.741 0.792 0.8 0.836 0.842 0.893 0.994 1.038 1.243 1.402 20140 18342 18310 16000 15110 12750 11500 13680 11700 12400 11150 11260 11430 11960 11330 12170 9000 11330 10410 11260 10890 10800 10900 11300 5400 5730 6680 8900 10300 8750 8200 9400 8150 8390 7850 8100 8380 8740 9070 9700 8500 8400 9000 9900 9100 8100 8100 8000 1.8 2.06 1.63 1.905 2.07 1.9 1.7 1.89 1.9 1.9 1.74 1.969 2.008 1.96 2.008 1.944 1.936 1.935 1.886 1.922 1.84 1.94 1.97 2 0.4 0.5 0.3 0.4 0.45 0.3 0.4 0.28 0.3 0.25 0.33 0.3 0.3 0.29 0.3 0.4 0.4 0.39 0.3 0.3 0.3 0.37 0.29 0.36 400 200 230 280 330 300 290 300 400 240 200 400 300 220 300 350 400 300 300 400 300 300 250 200 Singapore, 1 996, pp. 119-124 3. Pyalling A.A. et al, Int.J.of Thermophysics. 7 1001 (1998) 4. Ternovoi V.Ya., Filimonov A.S. et.al. in: Shock Compression of Condenced matter - 1997, ed. By S.C.Schmidt et.al., AIP Conference proceedings 429, NY, 1998, pp. 87-90. 5. .Ebeling W., Foerster A., Fortov V., Gryaznov V., Polischuk A. Thermophysical properties of hot dence plasmas, Shtuttgart - leipzig: Teubner, 1991, pp.142-172. 6. Ternovoi V.Ya., Filimonov A.S. et.al. in: Shock Compression of Condenced matter - 1999, ed. By M.D.Furnish et.al., AIP Conference proceedings 505, Melville, NY, 2000, pp. 189-192. 7 V. E. Fortov and I. V. Lomonosov. J. Pure & Appl. Chem. 69(4), 893-904 (1997). 8 Semenchenko V.K. Selected chapters of theoretical physics. Moscow: Education, 1966, pp 94. 9. Lienhard J.H., Chemical Engeneering Science 31, pp. 847-849(1976) = 0.9± O.lGPa . Tcr.p. = 9100 ± 200 K. cy of Tcr.p. depends on spinodal model Jnfortunately, in this method it's impossible to find1 r'ritir'dl HAncitx/ Tr\ ActimatA \7r-r n it'c necessary to trace isoentrope in wide pressure range from Hugoniot to critical pressure, and calculate Riemann's integrals, and accuracy of such great investigation wouldn't be sufficient. ACKNOWLEDGEMENTS The research described in this publication funded by part from RFBR grants 00-02-17750 and 01-02-06243. REFERENCES 1. Fortov, V.E., Lebedev M.E., Ternovoi V.Ya., Rev.Gen.Therm. Fr. 371, 589-591 (1992) 2. Ternovoi v.Ya., Fortov V.E., et.al. in: Physics of Strongly Coupled Plasmas, ed.by W.D.Kraeft et.al., World Scientific Publishing Co Pte Ltd, 62
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