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 TEMPERATURE MEASUREMENTS OF SINGLE AND DOUBLE SHOCK COMPRESSED LIQUID NITROGEN IN OVERTAKING SHOCK WAVE CONFIGURATION Alexei A.Pyalling, Vladimir Ya.Ternovoi, Alexander S.Filimonov Institute for Chemical Physics Research RAS, Chernogolovka, 142432, Russia. Abstract. In the present work the results of experiments on multiple shock compression of liquid nitrogen are presented. It was suggested to use two step compression waves to determine temperature of double compressed nitrogen not using window material. The proposed method can be used to determine optical densities of shock compressed material and phase-transformation boundaries with high accuracy. The abnormal speed of the secondary compression wave was registered after single compression to 40 GPa in nitrogen. The transport cross section of the electron-ion interaction in shock-compressed liquid nitrogen was estimated. INTRODUCTION of sound, and compressibility of the material at shock compression [7] The behavior of nitrogen under extreme conditions have been studied in theoretical and in experimental works. The simplicity of structure and absence of difficult chemical transformations allows one to create its equation of state iteratively, taking into account additional physical effects. In previous work [1] nitrogen was investigated at relatively low pressures of shock compression ( P < 40 GPa ), where it was appropriate to describe its behavior in the model of molecular liquid [2]. However this theory was unable to describe experiments [3,4] when nitrogen was compressed up to the pressure of 80 GPa. This required the inclusion of additional physical effects connected with dissociation [5] in the model. In the subsequent experiments [6] on double shock compression of nitrogen was register the effect of "shock cooling". After the reflection of a shock wave in nitrogen from a sapphire window, the sharp decrease of emission intensity was observed. Registered temperature dropped from 8-9 TK in the single compression wave, to 7-8 TK in double-compressed wave. It is possible to calculate the heat capacity of the material having measured the temperature, speed c uv 2 (D-U) —_______U ———————————— where D(U) is the shock wave velocity, U is the mass velocity, and y is the Griineisen coefficient. If there are no anomalies on the shock Hugoniot, then D~a+bU, Ds>0, Dm<0, D>U; so, "shock cooling" means a negative Griineisen coefficient. However, the use of a window material for creating the doubleshocked states of nitrogen allows one to attribute the diminishing of optical emission to the loss of transparency by sapphire window compressed to a pressure of ~ 70 GPa. The aim of the present work was to conduct experiments allowing us to prove the presence or absence of anomalies in the behavior of nitrogen in the area of the phase diagram. These data is of interest also for the development of equation of state of hydrogen, since the same physical models are used for describing these substances. 95 moment of rapid decrease of temperature) and to determine its optical thickness more accurately then in configuration A. The optical thickness of the target material is determined according to the time of increase of emission from the shock-wave front (from zero level to the stationary value). The time of emission increase from the shock wave front is influenced significantly by the geometry of the striker plate (striker is not always perfectly flat) forming the preshock wave, so there are always questions about the correct interpretation of the data observed. In configuration B the parameters of the layered system were selected to create high temperature in the volume of the sample during the temperature decrease of the shock front after the arrival of release waves. Thus, the difference between the measured temperature and the calculated temperature of the shock wave front gives information about the optical thickness of the sample. EXPERIMENTAL SETUP The experimental assembly consisted of a steel container 20 mm in diameter (0.5 mm thick bottom) filled with liquid nitrogen. The upper side the container was closed by the sapphire window, through which we measured the emission intensity of nitrogen during compression. The container was immersed in a foam box surrounded by liquid nitrogen and cooled to the temperature T0=77 K. The cooled target container was filled with nitrogen of high purity. The temperature in the assembly was measured with a chromel-cupel thermocouple. The optical measurement configuration was as in [7]. [Configuration A EVALUATION OF EXPERIMENTAL DATA. The equation of state of nitrogen was constructed according to the referenced model [6]. This model, for the description of behavior of molecular phase of nitrogen, uses the variational model of soft spheres. The free energy is written in the form: FIGURE 1. Two experimental setups used to measure optical densities and temperatures of single and double shock compressed nitrogen; also shown is the pressure profile of nitrogen at a single time during shock-compression; temperatures are measured both in the case of non-transparent material and semi-transparent. Fpu^Fu+FiM+Fel where FU - free energy in an ideal gas approximation, Fei- electron component contribution to the free energy, ^int - part of free energy taking into account the interpartial interaction. The experiments utilized two different setups (Fig. 1). In the first (Config. A) the parameters of the layered system were chosen to generate two-step structure of the compression wave in nitrogen. The layer of initially liquid nitrogen was loaded by two shock waves with increasing intensities. Later a second shock wave caught up with the front of the first shock wave and formed a single front of strong unitary compression. In the case of semi-transparent materials it is possible to measure the temperature of a weak single compression wave, the temperature of double-shock compressed material and the temperature of an intense single shock compression. In this configuration it is also possible to evaluate the optical thickness of the material of interest. In Config. B (Fig. 1) it is possible to determine the sound velocity of shock-compressed nitrogen (the The dissociation of nitrogen molecules was taken into account by assuming ideal, non-interacting nuclear and molecular gases. From the condition of minimum free energy we obtain Fdis = min{l - x)F£* + 2xF^°m + F.m + xE& (V) + The quantity Edis(V) is calculated at T=OK and assumed to be temperature independent. Edis(V) was assumed to take the form 96 . j (y) = a 0 -fl 1 (V-V 0 ) z V<VQ V>V0 fo (V) = a 0 EXPERIMENTAL RESULTS AND DISCUSSION. 9 However, such construction of free energy of a system, without interactions between various subsystems causes an abnormal form of the "cold" curve (isotherm at temperature close to zero). At the pressure of "metallization" (atomic configuration is favorable, free energy of atomic and metal phase intersects) on the cold curve, there appears a sharp decrease of pressure. At non-zero temperatures this results in the formation of quasi-VanDerVaals loops, imitating the phase transition of first order. This effect can be eliminated by the introduction into the model of an additional parameter - occupation of state. We assume that the occupation of molecular phase varies from 1 at normal density (the hole system can as in molecular state, as in atomic state) to 0 - at density of metallization (the system can no longer be in a molecular state due to the large density). ^W = ***&)/ Edis(V)>o Three experiments in Config. A were conducted (double shock-compression of nitrogen in a single shock-wave). Two of them were done at relatively low compression, with a striker plate velocity of 5-6 km/c (Fig. 2). In the third experiment the striker was accelerated up to a velocity of 7.5 km/s in order to produce significant dissociation of nitrogen in the first compression wave (Fig. 4). 200 400 600 800 1000 Time, ns FIGURE 2. Experiments in configuration A. Experimental data, calculation of shock temperature and temperature to be measured. In the first experiments good agreement between theoretical and experimental temperature profiles was achieved. There is a good agreement in the initial compression temperature, temperature of the final, powerful single shock-wave compression, and the initial profiles of temperature increase. Agreement between measured and calculated temperature of double-shock compression is not as good. The sound velocity calculated from these experiments is in good agreement with theoretical calculation. In Config. B two experiments were done, with different initial velocities of the striker plate (Fig.3). There is a good agreement between the experimental and calculated release profiles. This indicates that the theory evaluates well the sound velocity of shocked nitrogen and its volume dependence. Also, the theory is good in predicting the tail of the release wave when the temperature on the shock wave front is lower then measured one, due to emission from the internal, hot layers of nitrogen. But the time of increase of the emission from the shock-wave front from zero to the stationary value (at the very beginning of the temperature profile) was predicted properly only for the experiment with lower shock-wave This construction provides smoothness and monotony of isotherms at the density of metallization and only slightly affects the behavior of isotherms far from this density. For all the experiments, ID gas-dynamic calculations were done, using the above experimental parameters. This allowed one to calculate temperatures on the shock- wave front, and in the volume of nitrogen. Also, to make a comparison with experimental temperature profiles, recalculation of emission intensity was performed taking into account the optical thickness of nitrogen. According to the classical theory, the absorption coefficient depends on the number of electrons, frequency of light and frequency of electron-atom interactions [8]: where m is the electron mass, c velocity of light, e is the electron charge, Ne and Na are the concentrations of electrons and atoms respectively, q is the effective frequency of electron-atom interactions, u is the mean velocity of electrons, and otT is the transport cross section of electron- atom interactions. Throughout, 0 tr was taken to be o tr = 4 A2. 97 parameters, due to the significant role of shape of striker plate (non-flatness of plate) in the second case. ferent processes. These results cannot be described using current model EOS of nitrogen, new physical effects may likely have to be included. 1000 • Optical length obtained from best fit of all experimental data X Optical length based on the temperature increase rate of the first shock wave front , J 100 Shock wave temp Recalculated temp Experiment 400 600 800 1000 10 6 1200 Time, ns FIGURE 3. Experiments in configuration B. Experimental data, calculation of shock temperature and temperature to be measured. The parameters of shock compression in the second experiment in configuration B were chosen to be the same as parameters of the first compression in the third experiment in configuration A (with high speed striker) (Fig. 4). The main difference between these two experiments was that in configuration B the nitrogen after single compression was unloading and in configuration A nitrogen was double shockcompressed after the initial single compression. 7 8 Temperature, 10 3K FIGURE 5. Calculated optical density of nitrogen. The results of optical length estimation of nitrogen from present experimental data are shown on Fig. 5. This work was supported in part by Russian Fund for Basic Researches Grant N 00-02-17550. The authors thank V. K. Gryasnov and N. A. Afanas'ev for their help. REFERENCES 18 16 Single shock formation 1. 14 £12 2. £ 10 I 8 3. 4> H Shock wave Temp Recalculated TempExperiment 4 2 100 200 300 400 500 Time, ns 600 4. 5. 700 FIGURE 4. Experiments in configuration A. High velocity. Single shock wave was not formed, contrary to the theory. Theory was satisfactory in predicting the release profile in configuration B and in predicting the sound velocity in nitrogen. On the other hand, it was unable to predict the time when the second shock wave overtakes the first one in configuration A. On the experimental profile there is no sharp increase in temperature, which can be attributed to this observation. 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