Assessment of Safety and Risk with a Microscopic Model of Detonation by C.-O. Leiber by C.-O. Leiber - Read Online

Book Preview

Assessment of Safety and Risk with a Microscopic Model of Detonation - C.-O. Leiber

You've reached the end of this preview. Sign up to read more!
Page 1 of 1

Winkler.

PROLOGUE

Classical Theories of Detonation, a Description of the State of the Art

The principles of detonation theory are based on Schuster’s [1] interpretation of Riemann’s [2] ideas for the behavior of shock waves in detonating gases, and have been later applied also to condensed explosives. These principles are:

• Macroscopic quasicontinuum laminar flow is approached.

• Plane-wave considerations and corresponding impedances are established.

• The jump discontinuity is independent of time, whereas the flow may be time dependent.

• Chemical reaction occurs completely and instantaneously within the detonation jump. Quantities are in thermodynamic equilibrium.

In the more recent past, developments in detonation theory have been accomplished by Becker [3], Zel’dovich [4], J. von Neumann [5], and Doring [6]. When speaking of this ZND-theory I refer to a steady state theory.

It is usually assumed that the origin of detonations is thermal. This means that shock compression induces a temperature increase in the volume, which results in a thermal decomposition that would drive the shock.

Many assumptions have been based on this classical ZND-theory, where the originators are not quite clear. This is best evidenced in the paper of W. C. Davis [7]: The basic idea should be their key insight was to take a shocked material’s temperature and pressure as givens and to concentrate on how chemical reactions in the shocked state proceeded. Doring [8] commented that this had never been his idea. He feels that this idea would be strange and misleading.

It must be noted that before 1940 physical detonation theories had been considered to be of only academic interest; no practical need for such a tool was seen because everything had been solved experimentally. In these early days, the science of explosives was concerned only with inventing and developing new ever-more powerful explosives. This process had been entirely in the hands of able chemists, who approached the synthesis problems through application of their own insight. Therefore, many crude chemical and physical ideas and tests, as well as some sophisticated ones, are still in use and can present dangerous situations. For example, Schmidt [9] used the thermohydrodynamic detonation model to calculate detonation properties in the 1920s. According to the chemist’s viewpoint, he believed in thermochemical limits of explosion properties. Even though bubble sensitization of explosive materials leading to detonation was known at that time, the German authority Chemisch-Technische Reichsanstalt (CTR) denied such a possibility [l0].

The most serious error seems to be that explosives behavior is taken to be only a matter of chemical reactions (kinetics). The chemists view any hazards in the context of chemical reactions, totally ignoring physical explosions. As we have seen fiom the Oppau-accident in 1921, which was not an ‘allowed’ explosion, we lack even today the tools to predict or avoid such risks, other than prior experience. After this catastrophe the government reported to the Reichstag as naively as did their American colleagues to their government after the Texas City catastrophe in 1947.

The first practical need for a physical detonation theory resulted from the development of atomic bombs, where knowledge of precise high velocity processes of explosively driven materials are essential. Using conservation principles in plane-wave terms it became possible to calculate with this theory the materials’ behavior under (regular) shock attack. So shock wave physics was born in terms of excellent engineering estimation methods. The classical detonation theories are described in several monographs [ll–16], and many computer codes have been developed since that time. In the following chapters I will outline some ideas in a rudimentary fashion. For the original goal of shock and detonation research, there had been no need to consider so-called ‘pathological’ situations in explosives behavior though there are many.

Some unsolved problems of detonation are:

1) Plane-wave concepts are used, although plane and wavy detonation fronts exist, along with dark waves, in the center of a charge.

2) Classical theory only addresses High Velocity Detonation (HVD), in which the detonation velocity exceeds 6 km/s, in spite of the fact that the first detonation velocities observed in nitroglycerine (NG) were < 2 km/s. This detonation process in NG, called Low Velocity Detonation (LVD), is not well understood, and its existence in solids was denied for a long time.

3) Auniversal detonation velocity gap between 2 – 2.5 and 6 km/s exists for condensed explosives of normal high densities. This phenomenon is neither understood nor generally recognized.

4) Deflagration to Detonation Transition (DDT) does exist. Working codes have been developed using simple assumptions. The physical origin of DDT is not clear, partly because in plane-wave terms always and invariably one-half of the energy is in compression and one-half in flow.

5) Detonation is considered to be a shock wave accompanied by a chemical decomposition, which means that chemical processes drive hydrodynamic events. This coupling process has been known since Becker’s days (the 1920s), but no explanation has been advanced up to the present.

6) If there is a reliable theory, one expects that a univalent detonation pressure should be determined from different and very precisely determined experimental data. This is not the case.

7) Von Neumann [6] suggested in his classical paper for the substantiation of the ZND-theory that particle velocities would probably be much more effective for initiation than the shock heating process. No discussion ever followed this suggestion.

No guidelines exist at present to explain either physical explosions or unexpected chemical explosions and their causes.

Based on the fact that so many irregularities of detonation are assumed to be puthologicul, Kamlet’s [17] statement characterizes the state of the art:

The lore of detonation chemistry andphysics is a composite of sound experimental evidence, anecdotes, apocryphal tales and large amounts of misinformation. The misinformation is often not recognized as such, arising sometimes from misinterpretation of experimental results or incorrect measurements and sometimes from deliberate inaccuracies. In the latter case, it has been convenient to accept and use certain assumptions or interpretations because they work. Often they work not because they are intrinsically correct, but rather because they contain convenient compensating errors.

This demonstrates that detonation was often treated as a ‘chef’s’, where the ‘chef’ decided about truth. This is probably best evidenced by the different interpretations of the same facts at different institutions in even a single country. This situation has not improved since the pioneering years of detonation development.

Another old (ignored) question has arisen in Becker’s original work on detonation physics for the German academic degree of ‘Habilitation’. Nernst, as a winner of the Nobel-prize for chemistry in 1920 and an explosives authority, considered the volume heating process to be inadequate. Instead he pointed out the importance of hot-spots. No detonation model has yet been developed from this initiation mechanism.

Therefore it is the intent of the following considerations, to suggest principles of a microscopic detonation model, where the macroscopic (classical) models get asymptotic solutions. Also, shortcomings of the macroscopic view will be evaluated. So it appears that the formerly pathological phenomena turn out to be natural results, which can be explained in acoustic terms. This rationale is counter to the theory of shock phenomena. But the first leading term in each shock expansion is based on acoustics. So something is missing whenever acoustical results are neglected. A hrther argument is that the impedances are linear acoustic terms, therefore there should be no linear shock impedances present - but they are.

In the end, my personal conviction is: Even in linear acoustics everything is so complicated that one must simplify the theory in order to develop the model. Some analogies to the difficulties may be understood by considering the history of the development of the gas laws based on the kinetic gas molecules as opposed to the thermodynamic version.

The ideas presented here are not all new but were developed over centuries. In the sense of Newton: If I have seen further, it is because I have stood on the shoulders of giants. Remember, for example, the first physical application of a resonator in the Neolithic period about 2400 B. C. in the Hypogeum of Malta, see Figure 1, and the recognition of the physical effects of particles (in the atmosphere) by Derham, 1708 [18]!

Figure 1 Oracle of Hypogeum of Malta. The Helmholtz-resonator (Dimensions: 180 1 volume, neck 0.2 m², length 5 cm, resonance frequency 91 Hz). The voice is augmented and distorted due to the transformation of the energy of flow to acoustic waves. (Kind permission of Briiel & Kjaer, Kopenhagen).

References

1. Schuster, A. Note to H. B. Dixon, Bakerian Lecture: On the Rate of Explosion in Gases. Phil. Trans. Roy. Soc. London A. 1893;84:152–154.

2. Riemann, B. Über die Fortpflanzung ebener Luftwellen von endlicher Schwingungsweite. Götting. Nachr. 1859:192–196. [Götting. Abh. VIII, p 243/265.].

3. Becker, R. StoRwelle und Detonation. Z. Physik 1922;8:321–362. Becker, R., Physikalisches uber feste und gasfdrmige Sprengstoffe. Z. tech. Physik. 1922:253.

4. Ya. B. Zel’dovich, Collected Scientific Papers, Nauka, Moscow, 1984.

5. J. von Neumann, Theory of Detonation Waves, OSRD-Rept. No 549, 1942.

6. Doring, W. Der Dmckverlauf in den Schwaden und im umgebenden Medium bei der Detonation, in Probleme der Detonation. Deutsche Akademie der Luftfahrtforschung, 1940/1941;421–436. Doring, W. iiber den Detonationsvorgang in Gasen. Ann. Physik 5. Folge. 1943;43:421–436.

7. W. C. Davis. The Detonation of Explosives, Scientific American (1987)5, p. 981105, in German: Die Detonation von Sprengstoffen, Spektmm der Wissenschaft (1987)7, p. 70/77.

8. W. Doring, Letter from 06.10.1987 to Dr. Rudi Schall.

9. A. Schmidt, Beiträge zur thermodynamischen Behandlung explosibler Vorgange, Z. ges. Schieβ- und Sprengstoffwes. 24 (1929)2,3,4, p . 41/46; 90/93; 97/101; 144/148, and later contributions.

10. J. F. Roth, Personal communication. 1975.

11. Zel’dovich, Ya.B., Kompaneets, A.S. Theory of Detonation. New York and London: Academic Press, 1960.

12. Zel’dovich, Ya.B., Raizer, Yu.P. Physics of Shock Waves and High-Temperature Hydrodynamic Phenomena. New York and London: Academic Press; 1966;Vol. I and 11.

13. Gruschka, H.D., Wecken, F. Gasdynamic Theory of Detonation. London: Gordon & Breach, 1972.

14. Fickett, W., Davis, W.C. Detonation. Berkeley, Los Angeles, London: University of California Press, 1979.

15. Mader, Ch.L. Numerical Modeling of Detonations. Berkeley, Los Angeles, London: University of California Press, 1979.

16. Nettleton, M.A. Gaseous Detonations, their Nature, Effects and Control. London, New York: Chapman and Hall, 1987.

17. M. J. Kamlet, Lectures on Detonation Chemistry, No 1, 9/1986

18. Derham, W.D. Experimenta & Observationes de Soni Motu, aliisque ad id attinentibus, factae. Phil. Trans, Roy. SOCL. London. 1708;26:2–36.

I

SHORTCOMINGS IN THE MACROSCOPIC PLANE-WAVE MODEL OF DETONATION

Description of the Physics

The plane-wave detonation model considers the impedance and therefore the sound velocity in the Chapman-Jouguet (CJ) compressed state to be independent of the shape of the pressure wave and of the diameter of the charge. A plane piston in motion leads to a plane detonation wave.

To test this assumption, linear acoustics is applied to the piston model of detonation in the CJ compressed state. This cannot be accomplished by classical exact solutions of the Huygens-Rayleigh integral for the piston as a plane membrane, because the pressure and impedance over the diameter depend on geometry and dynamics, which in this case means a wavelength λ (Fig. I-2 to I-4). The impedance becomes complex. In the case of high dynamics, the real plane-wave impedance is asymptotically obtained, but large pressure variations result from the location of the membrane. By contrast, smooth pressure fronts are obtained for low dynamics, where the impedance disappears.

Figure I-2 Impedance of the piston of diameter 2a of Figure I-1 in usual Gaussian terms of complex quantities.

Figure I-3 Impedance of the piston of diameter 2a of Fig. I-1 in polar notation. The modulus of the impedance is the radius vector to the appropriate diameter ka = 2πa/λ.

Figure I-4 Pressure distribution across the diameter of the piston, x is the distance from the center of the piston (Stenzel/Brosze with kind permission).

Thus, a plane piston in motion will not produce a plane pressure wave. The classical macroscopic approach of the piston model of detonation as laminar flow of a homogeneous reactive medium is not consistent in itself, because if each element of the piston radiates pressure waves, then no plane wave can be expected by the application of Huygens’ principle on the elements of the radiating membrane.

Plane-Wave Detonation

Starting from the experimental demonstration that plane detonation fronts exist, then the plane piston model of detonation has brought much progress. Its main advantage is that engineering approximations of detonation can be obtained by application of the conservation equations of mass, momentum and energy, assuming a homogeneous laminar flow and ignoring any phase transitions.

The conservation laws result in:

(I-1)

(I-2)

Also, the Chapman-Jouguet (CJ) condition for stability is used in the form

(I-3)

c is the sound velocity in the Chapman-Jouguet (CJ) compressed state. This is linked with the Equation of State (EOS) of the reaction products, which is the result of the conservation of energy.

A detonation proceeds through an explosive mixture with a velocity D. Initially the medium (density ρo) is at rest (particle velocity is zero) and has a pressure po, which is small in comparison to the detonation pressure p. In the reacted explosive the density has increased to ρ and the particle velocity is up, see Figure I-1.

Figure I-1 Classical steady state piston (diameter 2a) model of detonation. The plane piston (membrane) is driven by the CJ-particle velocity leading to a plane pressure wave propagation with detonation velocity D.

Rearrangement of Equations I-1 to I-3 leads to an expression for the shock impedance Z, which corresponds to the acoustic impedance (ρc)CJ of the shock-compressed medium in the CJ-state. This is the well-known plane wave impedance of acoustics, which depends neither on the diameter of the piston nor on the wave shape, i.e., it is always constant.

(I-4)

Plane-wave assumptions and this shock impedance are the key tools of classical shock- and detonation physics to calculate shock reflection and transmission, for example to evaluate the detonation pressure {Goranson, see [I-1]}.

It is assumed in the classical detonation model that a plane piston of diameter 2a in motion with the appropriate CJ particle velocity up drives a plane pressure front propagating with velocity D (Figure I-1). The pressure and corresponding particle velocity are linked by the plane-wave impedance, which is determined from the original density ρ0 and detonation velocity D. On the other hand, the local sound velocity c is not known by direct measurements, but is inferred from the equation of state (EOS). Practically, engineering approximations are obtained by adjusting this EOS to actual calibration measurements of an explosive. Therefore, such solutions are only valid for the appropriate range of composition and geometry for which the EOS has been determined. It is therefore hardly surprising that any conclusions drawn from this model have similar limited validity. For example, determination of the detonation pressure for a single explosive by different experimental methods leads to a wide range of values: 195 kbar [I-2], 268, 275, 289, 292, and 312 kbar [I-3]. The spread of values (117 kbar) is much greater than the statistical uncertainty in the measurements (ca. ± 5 kbar).

Acoustics of a Piston

Again we assume a piston of diameter 2a and velocity up, but now postulate that the velocity varies harmonically with a frequency f, so that the wave vector k = 2 πf/c = 2π/λ. Any area element of this piston is a pressure-radiating element. At a given point of observation the total pressure may be obtained by Huygens’ principle. The added parts from these area elements vary as the point of observation varies. If this point moves out of the axis of symmetry, the pressure contributions change accordingly. According to Rayleigh [I-4], Backhaus [I-5], Stenzel [I-6], and Stenzel/Brosze [I-7] one gets:

(I-5)

or in integral form [I-8,I-9]

(I-6)

where J1() and H1() are the first order Bessel and Struve functions, respectively.

In Figure I-2 and I-3, the impedance values are plotted in two different coordinates for various ka values. It is inferred from these figures that a plane-wave impedance, Re Z = ρc, is realized for large values of ka, and Im Z = 0 is realized asymptotically for ka ⇒ ∞ (for large arguments J1() ⇒ 0, and H1() ⇒ 2/π). Contrary to the plane-wave assumption in detonation theory, this impedance is diameter dependent in that this diameter is related to the dynamic quantity λ.

The exact calculation of this pressure distribution over the surface of the membrane we owe to Stenzel, and Stenzel/Brosze [I-6,I-7], see Figure I-4. The result is that a very approximate ‘plane’ wave at low pressure amplitudes is obtained only for low ka values,where the impedances are complex as shown in Figures I-2 and I-3. Large pressure variations at the location on the membrane result for larger ka-values.

Because the impedance of a real plane wave does not depend on the shape of the pressure or particle velocity function, we can not try for another non-harmonic function. Apparently one never gets plane-wave behavior [Im Z = 0, Re Z = ρc] and a plane pressure wave propagation by a plane motion of the piston simultaneously.

Discussion

The plane-wave detonation model assumes the impedance and therefore the sound velocity in the CJ-compressed state to be independent of the shape of the pressure wave and the diameter of the charge. Acoustic considerations show that this can not be true, even for a loss-free medium. This incredible result in applied acoustics was accepted only after direct experimental demonstration [I-10], [I-11] *. Furthermore, if losses and rate effects of the chemical reaction in the detonation zone are taken into account, then the corresponding complex sound velocities also come into play [I-12].

If these acoustical considerations hold, then they indicate that plane pressure waves can not exist, even though they may be readily observed experimentally. We believe that the considerations do hold, and therefore the plane wave model is at best a rough approximation.

*Publication of these results had been refused by six esteemed journals in the 80ies due to apparent absurdness. But the well-known acoustician Otto Brosze remembered the same controversies in the 20ies. Finally to settle the argument a 6-m plane membrane was attached at the walls of the Reichstelegrafenamt in Berlin, and no plane pressure field could be noted! Even after the measurements, the controversies continued for many years, and were finally forgotten!

References

Duff, R.E., Houston, E. Measurement of the Chapman-Jouguet Pressure and Reaction Zone Length in a Detonating High Explosive. J. Chem. Phys. 1955;23:1268/1273.

Hollenberg, G., Kleinhanß, H.-R., Reiling, G. Messung des Chapman-Jouguet-Druckes mit Röntgen-Absorption. Z. Naturforsch. 1981;36a:437/442.

Davis, W.C., Venable, D. Pressure Measurements for Composition B-3. In: Proc. 5th Symp. (Int.) Detonation. Office of Naval Research, ACR-184; 1970:13/21.

§302, Dover, New York, reprint 1945 Rayleigh, J.W.S. The Theory of Sound. 1896;Vol. II.

Backhaus, H. Das Schallfeld der kreisförmigen Kolbenmembran. Ann. Physik 5. Folge. 1930;5:1/35.

Stenzel, H. Über die akustische Strahlung von Membranen. Ann. Physik, 5. Folge. 1930;7:947/982.

Stenzel, Brosze, Leitfaden zur Berechnung von Schallvorgängen. 2nd edition. Springer; 1958.

L. Huber, Personal communication, 1982.

Abramowitz, M., Stegun, I.A. Handbook of Mathematical Functions, National Bureau of Standards. Appl. Math. Ser. 55. 1970.

O. Brosze, Personal communication, 1985.

Backhaus, H., Trendelenburg, F. Über die Richtwirkung von Kolbenmembranen. Z. techn. Physik. 1926:630/635.

Einstein, A. Schallausbreitung in teilweise dissoziierten Gasen. Sitzungsber. Preuss. Akad. Wiss. 1920:380/385.

II

IMPEDANCE MIRROR PHOTOGRAPHY OF H. DEAN MALLORY

Photographs of detonation fronts, the development of detonation, and their side views may be obtained by using the impedance mirror streak and framing camera technique of H. Dean Mallory [II-1], [II-2]. The principle of this technique is shown in Figure II-1.

Figure II-1 Arrangements of the impedance mirror technique of Mallory to obtain the structure of a detonation front.

This technique is based on the fact that Plexiglas shows some shock elasticity; and thus will not break instantaneously in a shock attack. Therefore, an impinging structured, inhomogeneous pressure stem produces characteristic fingerprints, which may be observed on the mirror-coated Plexiglas.

Interpretation of Impedance Mirror Photographs

If a constant plane-wave impedance exists, pressure and particle velocities are in phase and Mallory’s original interpretation fully applies. However, if the impedance varies, as will be described below, pressure and particle velocities behave differently. In contrast to the pressure imprint on the Plexiglas, which may change with time, the particle velocity may erode the Plexiglas surface irreversibly. This was discussed with H. Dean Mallory, and he remembered his investigations of the detonating mixture of hydrazine mononitrate/hydrazine, where only one picture had been published up to now [Ref. II-2]. This detonating mixture shows no detonation luminosity, and the detonation products are optically transparent.

Side-on framing camera snap shots at an exposure time of 0.6 μs and an interframe distance of 1.5 μs were taken with equipment shown schematically in Figure II-1b without mirror. Some of the photographs are shown in Figure II-2.

Figure II-2 A series of detonating 18-molal hydrazine mononitrate/hydrazine looking through the reaction gases at a backlight. The grid lines are on the back surface of the tank. The numbers give multiples of the inter-frame distances of 1.5 μs.

To find erosion patterns, if present, a blue (early state) and a red (later stage) film copy has been made from each exposure of Figure II-2. This enabled us to compare photos taken at different time intervals by copying the different color films together. The full addition of the colors produced white images, whereas the earlier situation appears in blue, and the later in red. In Figure II-3 this is shown for two different time intervals. Note that from Figure II-3 the early engraved structures do not disappear. Most probably the erosion of the particle velocity remains forever, so that quantity variations at later times cannot be detected. The Plexiglas erosions are captured on film [II-3].

Figure II-3 Wrong color photo

The common structures of the picture pairs appear in white. The engraved structure seems to remain when one compares figures II-3a and Fig. II-3b.

Fig. II-3a. The blue picture 10 (not shown in Figure II-2) is copied with the red picture 15.

Fig. II-3b. From Figure II-2 the blue picture 5 is copied with the red picture 15.

Impedance Mirror Photographs of Detonating Nitromethane

Nitromethane (NM) is the classical liquid explosive used to test detonation ideas. It was found that volume homogeneous thermal explosion describes the detonation behavior. In the classical view, a volume homogeneous shock heating process leads to a uniform plane-wave detonation. Diluted NM will not change the mechanism, provided that detonation is still possible.

In Figure II-4, a previously unpublished series of photographs by the late Dr. Mallory are shown of the side views of the NM-detonation with increasing acetone content. Close examination of these photographs shows that the fronts roughen with increasing acetone content. It is extremely difficult to understand how such behavior can result from a uniform isotropic shock heating process.

Figure I-4 Impedance mirror streak camera views.

All shots were plane-wave initiated by a 10.2 cm diameter booster and a 2.54 cm thick Comp. B pad.

(Unpublished result of Dr. H. D. Mallory.)

a) 100 % NM, 6.35-cm ∅, 45.7-cm length, reaction time ≈22 ± 3 ns.

b) 90/10 vol.% NM/acetone, 7.6-cm 0, 30.5-cm length.

c) 85/15 vol.% NM/acetone, 9.5-cm 0, 30.5-cm length.

d) 80/20 vol.% NM/acetone, 7.6-cm 0, 30.5-cm length.

e) 75/25 vol.% NM/acetone, 7.6-cm 0, 30.5-cm length.

By head-on photography of the detonation front, Mallory [II-4] has shown the transition from smooth to rough fronts with increasing dilution of NM with acetone (Fig. II-5).

Figure II-5 Framing camera views into the detonation fronts of NM with varying dilution with acetone (plane-wave initiated) from H. D. Mallory [II-4]. X has a real height of 3.2 mm. Exposure time 0.75 μs.

Figure II-6 shows this problem even more dramatically: An NM/acetone = 75/25 vol% charge of 5.75-in. diameter and 6-in. length has been initiated by a plane-wave generator. As is evident from the streak camera record, detonation started at the left side of the charge in approximately the middle, and the lower part of the charge followed somewhat later when a second detonation started there. Since boundary effects and rarefactions cannot affect the apparently inert regions between the two detonations, we cannot ‘explain’ this result in usual plane-wave terms.

Figure II-6 Streak-camera record of a detonating charge of NM/acetone = 75/25 vol.%, diameter 14.6 cm, 15.2 cm length, plane-wave initiated. (Unpublished result of H. D. Mallory.)

These findings are also supported by many Russian experiments [II-5], showing that the detonation front roughens with increasing dilution. Typically, the front of a detonating neat high explosive exhibited a front roughness of about 10−5 cm with a periodicity of about 5 × 10−4 cm.

Pimbley, Mader and Bowman [II-6] also investigated plane-wave generators both theoretically and experimentally. They concluded that significant gradients appear in compression behind the front across the diameter even though the wave-front is plane.

All these results indicate that the assumption of a plane-wave detonation model is an inadequate approximation for more sophisticated problems, especially on the microscale.

The paradox may be removed if we consider not a plane- but a spherical-wave model. This will be discussed in detail later in this book.

The reflecting light from a detonating liquid should be specular for a plane detonation, but in diluted detonating NM it was only partially specular, and showed some diffuse components arising from a small roughness, according to Zel’dovich, Kormer, Krishkevich and Yushko [II-7].

Using the setup shown in Figure II-7, a streak photograph of detonating NM/acetone 45/55 vol.% is shown in Figure II-8 that shows considerable roughness of the detonation front, but the same experiments on inert liquids (like hexane, water or methylene iodide) showed no patterns. The period of intense activity lasts only for about 1μs [II-4].

Figure II-7 Experimental set-up.(1) plane-wave lens, (2) booster explosive, (3) 3-mm Al-plate, (4) NM-tank, (5) mirror plane, (6) Plexiglas mirror substrate. (7 half-silver mirror. (8) light source [Ref. II-4]

Figure II-8 Overdriven wave in NM/acetone = 45/55 vol.% impacting on the impedance mirror [Ref. II-4].

Comparing all these results, one may puzzle on the many, widely varying manifestations of detonation phenomena. Six camera records of detonating NM/acetone 75/25 vol.% are shown in Figure II-9 with very different behavior: The initiating pressures ranged from strong overdrive (120 kbar) down to 83 kbar, which is the steady state detonation pressure of this composition. By an overdrive the detonation becomes ‘more normal’. The system behaves similar to liquid propellants, which exhibit large critical diameters. Mallory and Graham [II-8] suggested the use of an overdrive to investigate such systems on a smaller scale (e. g. postage-stamp-size, very small-scale tests). These photos are partly unpublished results of Dr. H. Dean Mallory. The comments are given in the legend of Figure II-9.

Figure II-9 Impedance mirror photographs of detonating NM/acetone = 75/25 vol.%. Top Fig. II-9a.: Tank 7-cm I.D., 3.8-cm long, booster P-40 + 2.5 cm Comp. B. Center: The same. Right: The same, but tank length was 15.2 cm.Bottom Fig. II-9b. Same as above, but 7.6-cm tank length. Center: Tank 10.2-cm o.d. 7.6-cm long, booster: P-40 + 12.75 mm Comp B. Right: Tank 5.7-cm I. D., 7.6-cm long, boosted with P-40 + 2.5 cm Comp. B.

We note an exotic characteristic here: Diluting NM with carbon tetrachloride instead of acetone does not change the critical diameter even in large dilutions {Kusakabe and Fujiwara [II-9]}. Their suggestion that there should be a relationship between the critical diameter and the reaction time means that the reaction time for NM/CCl4 systems should be independent up to 45 vol % CCl4 dilution. Impedance mirror photographs of Mallory [II-10], proved this assumption approximately correct. But the mechanism of the diluent is not understood.

Solid Explosives

Such structures are also found for solid explosives. Figure II-10 shows impedance-mirror photographs of detonating TNT as the detonation ‘front’ impinges the impedance mirror.

Figure II-10 Impedance mirror photographs of detonating TNT. (Unpublished result of H. Dean Mallory.)

More interesting is Figure II-11, where subsurface bubbles in detonating cast baratol

Figure II-11 Impedance mirror photograph of cast baratol on a polished 1.22-mm Cu-foil into Al/hexane tank. (Unpublished result of H. Dean Mallory.) Left: Cast baratol with subsurface bubbles, where the left one made a breakthrough, and the rings below the X are refraction patterns of another bubble. The height of X indicates 3.2 mm. Right: Magnification of the interesting part.

Figure II-12 Dark waves and interaction patterns on the detonation front in undiluted NM; 22-mm∅ glass tube with 1.6-mm walls, and length of 12.7 cm. Exposure time 0.8 μs. Unpublished result of H. Dean Mallory. A similar set was published in [II-13]. The time sequence is upper left to right, and the same for the lower sequence.

Figure II-13 shows a smear camera record of detonating NM/acetone = 80/20, where initiation occurred at the left lower part by a bubble. Convergent and divergent waves resulted. More details can be found in the original paper [II-13].

Figure II-13 Smear camera record (covering about 15 μs) of detonating NM/acetone = 80/20 vol% in a 55-mm i. d. glass tube. The detonation stopped after a run of 10 cm. Initiation occurred by a bubble at the left side, bottom [II-13].

Figure II-14 shows the consecutive detonation fronts after a run of 7.5 cm [II-13]. Smooth and rough detonation areas, separated by a dark wave, can be seen clearly. Chapter XX (Figure XX-6) shows models of the smooth/rough transition and a dark wave.

Figure II-14 Detonating NM/acetone = 80/20 vol.% in a 55-mm inside diameter glass tube after 7.5 cm wave run. These consecutive pictures had exposure times of 0.8 μs. The X was 3.2-mm high [II-13].

There is often the belief that dark waves are typical for small dimensions and/or explosive compositions that tend toward chemical inertness. However, dark waves can probably be produced in pure nitromethane in very long tubes of 50 m and/or more with diameters of 15 to 20 cm. Events are observed that indicate a weakening of detonation or even a transition to burning of nitromethane. A reinitiation was also observed.

Reaction and Pressure Centers

We discussed with Dr. Mallory the old question, whether pressure waves are really coupled with any chemical reaction. To find an answer, he developed an impedance-mirror technique that made possible simultaneous observation of flame fronts. He used the system sketched in Figure II-15: In a Plexiglas prism one side has been mirror coated and the other remained optically transparent, so that, using an angular mirror, both sides could be simultaneously observed by a framing camera. However, it was necessary to illuminate the impedance mirror side with an argon