Cynthia Bolme

High strain-rate plastic flow in Al and Fe

Thin Fe and Al foils were ramp-compressed over several to tens of ns timescales to study the time-dependence associated with the onset of plastic flow. Peak stress states of 15–200 GPa were achieved through laser ramp-compression where the strain rate was varied, shot-to-shot, between 106 to 108 s−1. Our data combined with data from other dynamic compression platforms reveals a strong correlation between the peak elastic precursor stress, σE, and the strain rate at the onset of plastic flow, ɛ·p. In fcc Al, phonon drag dislocation flow dominates above ɛ·p~103s-1 and σE ∼ 0.03 GPa where σE scales as ɛ·p0.43. By contrast, the Al alloy 6061-T6 exhibits a relatively weak dependency of σE with ɛ·p up to strain rates of ∼107 s−1. Our Fe data, reveals a sharp increase in σE at ɛ·p>5×106s-1. This is consistent with a transition in plastic flow to a phonon drag regime.

The elastic-plastic response of aluminum films to ultrafast laser-generated shocks

We present the free surface response of 2, 5, and 8 μm aluminum films to shocks generated from chirped ultrafast lasers. We find two distinct steps to the measured free surface velocity that indicate a separation of the faster elastic wave from the slower plastic wave. We resolve the separation of the two waves to times as short as 20 ps. We measured peak elastic free surface velocities as high as 1.4 km/s corresponding to elastic stresses of 12 GPa. The elastic waves rapidly decay with increasing sample thickness. The magnitude of both the elastic wave and the plastic wave and the temporal separation between them was strongly dependent on the incident laser drive energy.We present the free surface response of 2, 5, and 8 μm aluminum films to shocks generated from chirped ultrafast lasers. We find two distinct steps to the measured free surface velocity that indicate a separation of the faster elastic wave from the slower plastic wave. We resolve the separation of the two waves to times as short as 20 ps. We measured peak elastic free surface velocities as high as 1.4 km/s corresponding to elastic stresses of 12 GPa. The elastic waves rapidly decay with increasing sample thickness. The magnitude of both the elastic wave and the plastic wave and the temporal separation between them was strongly dependent on the incident laser drive energy.

Shock induced chemistry in liquids studied with ultrafast dynamic ellipsometry and visible transient absorption spectroscopy.

The response to ultrafast laser shock loading of nine liquids was monitored in an effort to reveal evidence of chemical changes occurring during the first 350 ps following the shock front. In an effort to compare molecular structures possessing a variety of common bonding patterns, data were acquired for the liquids: cyclohexane, cyclohexene, 1,3-cyclohexadiene, benzene, water, acetonitrile, acrylonitrile, tert-butylacetylene, and phenylacetylene. Transient absorption spectra were measured in the spectral region from 440 to 780 nm over shock stress states from 7 to 20 GPa. Ultrafast dynamic ellipsometry was used to measure the shock and particle velocity as well as the shocked refractive index. Significant transient absorption attributed to chemical reaction was observed for shocked phenylacetylene and acrylonitrile. Evidence of volume decreasing chemical reactions was also observed in the ultrafast dynamic ellipsometry data for phenylacetylene and acrylonitrile. The liquid 1,3-cyclohexadiene exhibited volume decreasing reaction in the ultrafast dynamic ellipsometry data but did not exhibit an increase in the transient absorption spectra. There was no evidence of chemical reaction in cyclohexane, cyclohexene, benzene, water, acetonitrile, or tert-butylacetylene in the first 350 ps, despite the application of shock stress that was in many cases well above the reaction threshold observed at microsecond time scales.

Single shot Hugoniot of cyclohexane using a spatially resolved laser driven shock wave

To develop a more efficient method of determining pressure dependent material response to shock loading, we used the spatial energy distribution of a shock generating laser beam to create a range of nearly one-dimensional stresses in a single laser shot. Ultrafast dynamic ellipsometry was used to measure the Hugoniot and shocked refractive index of cyclohexane subject to this shock loading.

Heterogeneous flow and brittle failure in shock-compressed silicon

We combine a recently developed high-resolution two-dimensional (2D) imaging velocimetry technique (velocity interferometer system for any reflector (VISAR)) with 1D VISAR measurements to construct a moving picture of heterogeneous deformation in shock-compressed single crystal silicon. The 2D VISAR takes an intensity snapshot of target velocity and reflectivity over a mm field-of-view while the compression history is simultaneously recorded by the 1D VISAR. Our data show particle velocity surface roughening due to the anisotropic onset of plasticity and, above ∼13 GPa, a structural phase transformation. Shock arrival at the Si free-surface is characterized by the formation of fracture networks and incipient velocity jetting.

The elastic tensor of single crystal RDX determined by Brillouin spectroscopy

The elastic tensor of 1,3,5-trinitroperhydro-1,3,5-triazine (also known as RDX, hexogen, and cyclotrimethylene trinitramine) was determined using Brillouin spectroscopy of as-grown single crystals. This study addresses inconsistencies in the literature between the elastic tensor measurements made using Brillouin spectroscopy in the GHz frequency range and the measurements using various techniques in the kHz-MHz frequency range. These Brillouin results are consistent with previous measurements made in the kHz-MHz frequency range using various techniques and are also consistent with velocity measurements at 15 GHz using picosecond acoustic interferometry. These results are in disagreement with the previously published elastic tensor determined using Brillouin spectroscopy, and there are differences of several percent amongst the consistent set of elastic tensor determinations. The origins of the disagreement and differences are discussed.

Ultrafast shock-induced chemistry in carbon disulfide probed with dynamic ellipsometry and transient absorption spectroscopy

We used transient visible/near-infrared absorption spectroscopy and ultrafast dynamic ellipsometry to characterize carbon disulfide (CS2) shocked with an ultrafast laser pulse. We found a volume-decreasing reaction, characterized by the deviation of the shock and particle velocity (us and up) points from the unreacted Hugoniot, above up = 1.5 km/s. This result contrasts with literature plate-impact data, which found the reaction-induced deviation from the unreacted Hugoniot to occur at up = 1.2 km/s. We attribute this disparity to the difference in timescale between plate-impact experiments (ns to μs) and our ultrafast experiments (sub-ns), as our ultrafast experiments require higher shock pressures and temperatures for an observable reaction. The volume-decreasing reaction was accompanied by a large increase in absorption of the reaction products, necessitating the use of impedance matching techniques to characterize the us-up points above the reaction cusp. Using transient absorption spectroscopy, we di...

Shock Hugoniot equations of state for binary ideal (toluene/fluorobenzene) and nonideal (ethanol/water) liquid mixtures.

Laser shock Hugoniot data were obtained using ultrafast dynamic ellipsometry (UDE) for both nonideal (ethanol/water solutions with mole percent χ(ethanol) = 0%, 3.4%, 5.4%, 7.5%, 9.7%, 11%, 18%, 33%, 56%, 100%) and ideal liquid mixtures (toluene/fluorobenzene solutions with mole percent χ(toluene) = 0%, 26.0%, 49.1%, 74.9%, 100%). The shock and particle velocities obtained from the UDE data were compared to the universal liquid Hugoniot (ULH) and to literature shock (plate impact) data where available. It was found that the water UDE data fit to a ULH-form equation suggests an intercept of 1.32 km/s, lower than the literature ambient sound speed in water of 1.495 km/s (Mijakovic et al. J. Mol. Liq. 2011, 164, 66-73). Similarly, the ethanol UDE data fit to a ULH-form equation suggests an intercept of 1.45 km/s, which lies above the literature ambient sound speed in ethanol of 1.14 km/s. Both the literature plate impact and UDE Hugoniot data lie below the ULH for water. Likewise, the literature plate impact and UDE Hugoniot data lie above the ULH for ethanol. The UDE Hugoniot data for the mixtures of water and ethanol cross the predictions of the ULH near the same concentration where the sound speed reaches a maximum. In contrast, the UDE data from the ideal liquids and their mixtures are well behaved and agree with ULH predictions across the concentration range. The deviations of the nonideal ethanol/water data from the ULH suggest that complex hydrogen bonding networks in ethanol/water mixtures alter the compressibility of the mixture.

Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics

High explosives that are photoactive, i.e., can be initiated with light, offer significant advantages in reduced potential for accidental electrical initiation. We examined a series of structurally related tetrazine based photoactive high explosive materials to detail their photochemical and photophysical properties. Using photobleaching infrared absorption, we determined quantum yields of photochemistry for nanosecond pulsed excitation at 355 and 532 nm. Changes in mass spectrometry during laser irradiation in vacuum measured the evolution of gaseous products. Fluorescence spectra, quantum yields, and lifetimes were measured to observe radiative channels of energy decay that compete with photochemistry. For the 6 materials studied, quantum yields of photochemistry ranged from <10(-5) to 0.03 and quantum yield of fluorescence ranged from <10(-3) to 0.33. In all cases, the photoexcitation nonradiatively relaxed primarily to heat, appropriate for supporting photothermal initiation processes. The photochemistry observed was dominated by ring scission of the tetrazine, but there was evidence of more extensive multistep reactions as well.

Shock Hugoniot equations of state for binary water-alcohol liquid mixtures

Shock Hugoniot data were obtained using laser generated shock and ultrafast dynamic ellipsometry (UDE) methods for several non-ideal water-alcohol liquid mixtures, with the alcohols being methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, and t-butanol (a.k.a., 2-methyl-2-propanol or tert-butanol). The sound speeds of the mixtures were obtained using Brillouin scattering when not available in the literature. The shock and particle velocities obtained from the UDE data were compared to expectations of the universal liquid Hugoniot (ULH) and to literature shock (plate impact) data where available. The ethanol/water data were presented in a previous publication [Schulze et al., J. Phys. Chem. A 117, 6158–6163 (2013)]. The shock Hugoniot trends for all these mixtures, here represented as deviations from predictions of the ULH, versus fraction of alcohol are quite similar to each other and suggest that complex hydrogen bonding networks in alcohol-water mixtures alter the compressibility of the mixtures.