Publications

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The performance and sensitivity of aged composite explosives based on the epsilon polymorph of hexanitrohexaazaisowurtzitane (ϵ-CL-20) have been evaluated with the laser-induced air shock from energetic materials (LASEM) technique using only milligram quantities of material. The LASEM results demonstrated reduced explosive performance (i. e., lower estimated detonation velocities) and higher sensitivity to ignition with increasing ageing. Chemical analysis of the explosive formulation subjected to ambient and accelerated aging was conducted to help understand the LASEM results. The Fourier Transform Infrared (FTIR) spectra revealed no evidence for conversion to lower-energy polymorphs. Based on the desorption gas chromatography/mass spectrometry (D-GC/MS) results, the observed decrease in performance and increase in sensitivity for the explosive powder aged at 100 °C (relative to ambient and 70 °C aging) have been attributed to changes related to solvent inclusions in the molding powders.

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Pentaerythritol tetranitrate (PETN) is a common secondary explosive and has been used extensively to study shock initiation and energy propagation in energetic materials. We report 2D IR measurements of PETN thin films that resolve vibrational energy transfer and relaxation mechanisms. Ultrafast anisotropy measurements reveal a sub-500 fs reorientation of transition dipoles in thin films of vapor-deposited PETN that is absent in solution measurements, consistent with intermolecular energy transfer. The anisotropy is frequency dependent, suggesting spectrally heterogeneous vibrational relaxation. Cross peaks are observed in 2D IR spectra that resolve a specific energy transfer pathway with a 2 ps time scale. Transition dipole coupling calculations of the nitrate ester groups in the crystal lattice predict that the intermolecular couplings are as large or larger than the intramolecular couplings. The calculations match well with the experimental frequencies and the anisotropy, leading us to conclude that the observed cross peak is measuring energy transfer between two eigenstates that are extended over multiple PETN molecules. Measurements of the transition dipole strength indicate that these vibrational modes are coherently delocalized over at least 15-30 molecules. We discuss the implications of vibrational relaxation between coherently delocalized eigenstates for mechanisms relevant to explosives.

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We present the results of an LDRD project to develop diagnostics to perform fundamental measurements of material properties during shock compression of condensed phase materials at micron spatial scales and picosecond time scales. The report is structured into three main chapters, which each focus on a different diagnostic devel opment effort. Direct picosecond laser drive is used to introduce shock waves into thin films of energetic and inert materials. The resulting laser - driven shock properties are probed via Ultrafast Time Domain Interferometry (UTDI), which can additionally be used to generate shock Hugoniot data in tabletop experiments. Stimulated Raman scattering (SRS) is developed as a temperature diagnostic. A transient absorption spectroscopy setup has been developed to probe shock - induced changes during shock compressio n. UTDI results are presented under dynamic, direct - laser - drive conditions and shock Hugoniots are estimated for inert polystyrene samples and for the explosive hexanitroazobenzene, with results from both Sandia and Lawrence Livermore presented here. SRS a nd transient absorption diagnostics are demonstrated on static thin - film samples, and paths forward to dynamic experiments are presented.

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We present the results of a two year early career LDRD project, which has focused on the development of ultrafast diagnostics to measure temperature, pressure and chemical change during the shock initiation of energetic materials. We compare two single-shot versions of femtosecond rotational CARS to measure nitrogen temperature: chirped-probe-pulse and ps/fs hybrid CARS thermometry. The applicability of measurements to the combustion of energetic materials will be discussed. We have also demonstrated laser shock and particle velocity measurements in thin film explosives using stretched femtosecond laser pulses. We will discuss preliminary results from Al and PETN thin films. Agreement between our results and previous work will be discussed.

We discuss recent experiments and modeling for the chirped-probe-pulse generation of single-laser-shot femtosecond pure-rotational CARS/CSRS spectra from room-temperature gases. A pure-rotational Raman coherence is impulsively generated using near-transform-limited femtosecond pump/Stokes excitation, and the coherence is probed by stretching a nominally 100-fs near-transform-limited probe beam to approximately 1.7 ps via the refractive-index dispersion in a 30-cm long flint-glass rod. The linearly chirped probe spectrum and phase beat against the time-dependent Raman polarization to generate complex spectra. Chirped-probe-pulse rotational CARS/CSRS offers an interesting alternative to hybrid fs/ps rotational CARS, in which a band-limited pulse of limited energy is used, because all of the available probe pulse energy can be retained in a chirped-probe-pulse experiment. Our early chirped-probe spectra are presented and the details of our initial model calculations are provided. The temperature sensitivity of the chirped-probe results is illustrated using calculated spectra.

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