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 DETONATION PHENOMENA OF PBX MICROSAMPLES I. Plaksin, J. Campos, J. Ribeiro and R. Mendes Laboratory of Energetics andDetonics, Mech. Eng. Dep., Faculty of Sciences and Technology, University ofCoimbra, Polo II, 3030 Coimbra, PORTUGAL Abstract. Detonation study of PBX micro-samples, based in HMX with an inert (HTPB, epoxy) or energetic (GAP) binder was performed on the meso-scale level, using the multifiber optical probes of 50 Jim of maximum resolution, connected directly to a fast electronic streak camera with 0.6 ns resolution. The direct 2D observation of particle to particle successive transition of transmitted shock wave, through the binder, allows to analyse and to discuss, not only the cooperative formation of a multihead detonation front (DF), in the collection of particles surrounded by binder, but also the synenergetic effect, behind the DF, by the appearing of dissipative structures drawing spatial and temporal DF oscillations. main different kinds of detonation wave [DW] regimes, showing different unsteady spatialtemporal dissipative structures [DS]. These spatial-temporal DS are consequently the OS with the transversal SW (represented the cellular DW with the longitudinal-transversal DF oscillations) and OS without transversal waves, but with the additional longitudinal shocks (DF as a oscillating giant monocell). Characteristic sizes of DS depend on the EM physical/chemical properties and its rheology. We have detected both of these regimes in PBX *~3. The phenomenology of the origination and transformation of naturally unstable PBX detonation regimes has been already described 6 , based on the experiments on the meso-scale level. The factor of divergence of the reactive flow behind the FF (specified by front curvature) was found to be the influent parameter determining the regimes of DW instabilities and DS. It is obvious that the increase of the divergence, in the reacting particles flow, will change the rate of relaxation, in strongly non-equilibrium temperature/stress fields, behind the FF. Micro-mechanisms of temperaturestress transfer are very important in the OS lateral phase formation. The kinetic relaxation level, in the INTRODUCTION Phenomena of pulsing detonation of PBX was originally mentioned *~3 in the experiments, carried out on the meso-scale level, as a result of the application of high resolution multi channel optical method, based on optical fiber strip1"3. Phenomena of pulsing detonation, in chemically reacted media, implies that the initially smooth shock front, induced by the external source, losses its stability and it is followed by the origination of the oscillating structure [OS], behind the forward front [FF]. OS appears as a result of the inter-influence, in the strongly non equilibrium zone within the FF and chemical reaction zone [CRZ], of a few relaxation phenomena: kinetic relaxation involving release of energy (due to the exothermic reactions), thermal dissipation (due to heat/mass transfer) and stress relaxation (due to the existing limit velocity of impulse/shock waves [SW] propagation). Theoretically it was obtained4'5 that, independently of the physical nature of the energetic material, but according to the combination of different main relaxation times, in energy release and heat/mass transfer, and under the influence of the fluctuations), it can exist two 918 process of propagation in crystals of shock reactive wave [SRW], constitutes the governing factor determining the initial phase of OS origination. The existing delay of the energy release, in shocked and reacting crystals (in PBX, after the FF), could imply the changing of process of energy transfer and the pattern of non equilibrium temperature and stress fields, in CRZ. The presented study concerns the evaluation of the relaxation phenomena of energy release and of the stress fields, associated with SW propagation in explosive crystals, by the direct registration of SW within single crystals and its clusters, under the similar conditions to the PBX detonation. This objective also implies the clarification of the complex pattern of the OS depending not only by particle sizes and its compaction but also by the binder nature (inert or reactive). EXPERIMENTS The experiments were carried out on the mesoscale level with the micro and mini samples of PBX, based on HMX crystals surrounded by polymer binders (HTPB, epoxy, GAP) or by water. The multifiber optical probes [MFOP] of the matrix type, with 250 um of spatial resolution (50 pm maximum, in colimation mode)7, were connected directly to a fast electronic streak camera (THOMSON TSN 506N). The streak records, with 0.6 ns of maximum temporal resolution, allow the 2D and 3D analysis of SW and DW in PBX microsamples and HMX crystals. This procedure allows the registration of, not only the emitted irradiation from the front surface (in SW propagation inside the p-sample), but also the induced stress amplitudes and the front geometry (in thin layers of kapton), from the input and output SW. 1.5 2 Z(mm) 2.5 0 50 100150 Intensity of light (%) f) g) FIGURE 1. Registration on the SW propagation in HMX crystal, surrounded by HTPB binder, [a) experimental set-up; b); c); and d) micro-photos of HMX crystal, matrix MFOP and the MFOP in the background of the crystal; e) photochronogram; f) z-t diagram and velocity of SW before, during and after the crystal; g) histogram of the relative intensity of the light emitted from the central zone of the propagated S W front. The experimental results, presented in these figures, show the significant effects of the SW propagation inside the HMX crystal: 1 - The non monotonous built up and following decrease of SW velocity D, in order of the successive increasing and decreasing of the crystal cross section, followed by the enhance of the light emission intensity, at the end of the SW run. Pike of D corresponds to 2/3 of SW total run in the crystal; 2 - The delay time of the maximum stress phase, in the down kapton barrier, corresponding to the delay of the pike of energy release.; 3 - Anisotropical effect of the SF propagated through the binder, with the enhanced stress, not in the central, but in the preferential zone of the crystal/binder interface, proved by preferential development of SW in kapton barrier (Figure 2 e)). RESULTS AND DISCUSSION Non Monotonous Shock Reaction and Energy Release in Coarse HMX Crystals Two experiments have been conducted for the direct time registration of the SW propagation in single coarse HMX crystals, surrounded HTPB binder (Figure 1) and by water (Figure 2). 919 FIGURE 2. Experiment with HMX crystal, surrounded by water, a) experimental set-up, b) HMX crystal and side MFOP, c) HMX crystal and the bottom MFOP, top view d) photo-chronogram showing the pulsing SW propagation inside the crystal, e) detail of the obtained photo-chronogram (bottom MFOP), showing the surface edge effect of the enhanced SW propagation in the peripheral zone of crystal. 1.5 FIGURE 3. Experiments with vertically oriented group of three HMX crystals in epoxy binder, a) experimental set-up; b) HMX crystals and side MFOP; c) photo-chronogram showing the pulsing SW propagation; d) z-t diagram of SW propagation from crystal to crystal. The obtained results clarify the mechanism of relaxation of the HMX crystal reaction, induced by strong SW, proving the existing time delay in its energy release, behind the FF. The experimental time relaxation seems to be greater than the time needed for the shock propagation inside the crystal6. Future developments will be focused to the quantitative evaluation of the ratio relaxation time vs. ignition delay. The results of the experiment with the vertical group of three HMX crystals, in the epoxy binder, are presented in Figure 3, showing the non monotonous (pulsing) process of the SW propagation, inside the crystals, and its transition from crystal to crystal, through the 10-20 pm thick inter-particle space. The mean velocity of SW propagation, inside the crystal's chain is estimated in 7.0 mm/ps, that exceeds in ~1.4 times the SW velocity in the surrounding epoxy binder (but in —1.2 times less than the maximum velocity within the individual crystals). From the presented results it can be concluded that the defined relaxation effect of the unstable kinetics of shock reaction of a single crystal, accompanied by the surface edge effect, shows the same essential properties that can be observed in the group of crystals, creating the conditions for high order of fluctuations of energy dissipation, behind the FF, followed by formation of the DS by the mechanism of the transversal micro shock interactions. Reactive Waves Propagation, Interaction and Transition in the Ensemble of HMX Crystals These kind of experiments were performed with a collection of crystals, arranged in the vertical position, related to the initiating SW. Other results of experiments with horizontal clusters of HMX crystals, surrounded by HTPB and by GAP binders, show3 the significant role of the binders nature in the interaction process between the induced SW in the inter-crystal space. Performed tests show colliding SW's, generating the strong reaction in GAP binder, generate a multi-head front less fluctuated (more homogeneous) that appears with the HTPB binder. 920 These experimental results confirm the synergetic effects in PBX detonation described in the past3'6. //Kapton 7 5 0 jim 100 jim CONCLUSIONS Matrix of MFOP ,„„„. 4x20 fibers To THOMSON TSN 506 N The detonation study of PBX on the meso-scale level has been carried out applying the highresolution multi-fiber optical technique, in original tests, with single, two and more particles, surrounded by inert and energetic binders. The obtained results show the kinetic instability in shock reaction of coarse HMX crystals, surrounded by binder, the cooperative formation of a multihead detonation front (DF), in the collection of particles, and also the synergetic effect, behind the DF, by the appearing of dissipative structures with spatial and temporal DF oscillations. FIGURE 4. Long Channel Test (80x5x5mm, PBX charge in copper confinement) with PBX micro sample in its terminal zone, a) terminal detail of experimental setup; b) photochronogram showing the existing of the cellular structure of DF and OS. TTT PB 1.06 mm Kapton Barrier -Linear MFOP To Thompson REFERENCES TSN-506N FIGURE 5. Mini Gap Test, a) experimental setup; b) photochronogram. 1. Plaksin, L, Campos, J., Mendes, R., and Gois, J., "Interaction of Double Corner Turning Effect in PBX", Shock Compression in Condensed Matter 1997, edited by S. C. Schmidt, D. P. Dandekar, and J. W. Forbes, AIP CP 429, New York, 1998, p.p. 755758 2. Plaksin, L, Campos, J., Mendes, R., Ribeiro, J., and Gois, J., "Pulsing Behaviour and Corner Turning Effect of PBX", in Eleven International Symposium on Detonation, pp. 679-685. 3. Plaksin, J. Campos, R. Mendes, J. Ribeiro and J. Gois, "Mechanism of Detonation Wave Propagation in PBX with Energetic Binder", Shock Compression in Condensed Matter - 1999, edited by M. D. Furnish, L. C. Chhabildas, and R. S. Hixon, AIP CP 505, New York, 2000, p.p. 817-820 4. Daniljenko, V. A., Kudinov, V. M., Dokladi. Akademii Nauk Ukr. SSR, 1982, N. 12, p.p. 24-27 5. Daniljenko, V. A., Dissertation. Institute of Hydrodinamics of Siberian Branch of Academy of Sciences of USSR. 1984. Experiments with micro and mini samples of PBX The experiments, demonstrating the selforganization phenomena in PBX detonation, were carried out with p-samples and m-samples of PBX based on 82 mass percent of HMX (80% of d50 = 240 pm, 20% d50 = 17 pm) and 18% of an energetic binder (GAP). The results of the long channel test6 (where DF has a big positive curvature) show the existence of the DS forming the multi-head, or cellular DF, and the process of their origination and development after the DF had propagated through a kapton p-barrier. The characteristic size of the individual cell is equal to 5-6 d50 of coarse HMX particles. The results of mini-gap test6 (Figure 5) with the quasi-plane SW input, shows the existence of the longitudinal oscillations of DF, representing in this case a giant mono-cell. Its origin is immediately after the shock run equal to 2xd50. 6. Plaksin, L, Campos, J., Ribeiro, J., and Mendes, R., "Irregularities of Detonation Wave Structure and Propagation in PBX", 32nd International Annual Conference of ICT - Energetic Materials, Ignition Combustion and Detonation, Karlsruhe, July 3-6, 2001, pp. 31-1 to 31-14. 921
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