Robert Scharff

Determining the refractive index of shocked [100] lithium fluoride to the limit of transmissibility

Lithium fluoride (LiF) is a common window material used in shock- and ramp-compression experiments because it displays a host of positive attributes in these applications. Most commonly, it is used to maintain stress at an interface and velocimetry techniques are used to record the particle velocity at that interface. In this application, LiF remains transparent to stresses up to 200 GPa. In this stress range, LiF has an elastic-plastic response with a very low (<0.5 GPa) elastic precursor and exhibits no known solid-solid phase transformations. However, because the density dependence of the refractive index of LiF does not follow the Gladstone-Dale relation, the measured particle velocity at this interface is not the true particle velocity and must be corrected. For that reason, the measured velocity is often referred to as the apparent velocity in these types of experiments. In this article, we describe a series of shock-compression experiments that have been performed to determine the refractive index of LiF at the two most commonly used wavelengths (532 nm and 1550 nm) between 35 and 200 GPa to high precision. A modified form of the Gladstone-Dale relation was found to work best to fit the determined values of refractive index. In addition, we provide a direct relationship between the apparent and true particle velocity to correct experimentally obtained wave profiles by others using these velocimetry techniques.

Coherent control of multiple vibrational excitations for optimal detection

While the means to selectively excite a single vibrational mode using ultrafast pulse shaping are well established, the subsequent problem of selectively exciting multiple vibrational modes simultaneously has been largely neglected. The coherent control of multiple vibrational excitations has applications in control of chemistry, chemical detection and molecular vibrational quantum information processing. Using simulations and experiments, we demonstrate that multiple vibrational modes can be selectively excited with the concurrent suppression of multiple interfering modes by orders of magnitude. While the mechanism of selectivity is analogous to that of single mode selectivity, the interferences required to select multiple modes require complicated non-intuitive pulse trains. Additionally, we show that selective detection can be achieved by the optimal pulse shape, even when the nature of the interfering species is varied, suggesting that optimized detection should be practical in real world applications. Experimental measurements of the multiplex coherent anti-Stokes Raman spectra (CARS) and CARS decay times of toluene, acetone, cis-stilbene and nitromethane liquids are reported, along with optimizations attempting to selectively excite nitromethane in a mixture of the four solvents. The experimental implementation exhibits a smaller degree of signal to background enhancement than predicted, which is primarily attributed to the single objective optimization methodology and not to fundamental limitations.

Sound speed measurements in tantalum using the front surface impact technique

Shock compression experiments were performed on tantalum to determine the longitudinal sound speed on the Hugoniot from 36 to 105 GPa. Tantalum samples were impacted directly on to lithium fluoride windows at velocities ranging from 2.5 to 5.0 km/s and the resulting particle velocity profiles at the sample/window interface were recorded using optical velocimetry techniques. The time of arrival of the rarefaction wave from the back surface of the tantalum sample was then used to determine the longitudinal sound speed at the corresponding impact stress. In contrast to recently reported work, we see no evidence of a phase transition in the tantalum in this stress range.

Use of the Gerchberg–Saxton algorithm in optimal coherent anti-Stokes Raman spectroscopy

AbstractWe are utilizing recent advances in ultrafast laser technology and recent discoveries in optimal shaping of laser pulses to significantly enhance the stand-off detection of explosives via control of molecular processes at the quantum level. Optimal dynamic detection of explosives is a method whereby the selectivity and sensitivity of any of a number of nonlinear spectroscopic methods are enhanced using optimal shaping of ultrafast laser pulses. We have recently investigated the Gerchberg–Saxton algorithm as a method to very quickly estimate the optimal spectral phase for a given analyte from its spontaneous Raman spectrum and the ultrafast laser pulse spectrum. Results for obtaining selective coherent anti-Stokes Raman spectra (CARS) for an analyte in a mixture, while suppressing the CARS signals from the other mixture components, are compared for the Gerchberg–Saxton method versus previously obtained results from closed-loop machine-learning optimization using evolutionary strategies. FigurePhoto of an acousto-optic modulator based pulse shaper, with red lines denoting the laser beam path. Entering at the bottom left is the transform limited pulse (spectrogram inset shows wavelength versus time in a false color plot), and exiting at the bottom right is the the arbitrarily shaped pulse

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.

Systematics of Compaction for Porous Metal and Metal-Oxide Systems

The effects of particle morphology and initial density is examined with respect to the shock densification response of initially porous metal (Cu) and metal-oxide (CeO2) materials. Specifically, the ability of a continuum-level compaction model to capture the measured densification trends as a function of initial density and particle morphology are investigated. Particle morphology is observed to have little effect on the densification response of both Cu and CeO2, while initial density appears to have a stronger effect. In terms of continuum-level compaction strength, Cu and CeO2 exhibit dissimilar trends.

Optimal coherent control methods for explosives detection

We are utilizing control of molecular processes at the quantum level via the best capabilities of recent laser technology and recent discoveries in optimal shaping of laser pulses to significantly enhance the detection of explosives. Optimal dynamic detection of explosives (ODD-Ex) is a methodology whereby laser pulses are optimally shaped to simultaneously enhance the sensitivity and selectivity of any of a wide variety of spectroscopic methods for explosives signatures while reducing the influence of noise and environmental perturbations. We discuss here recent results using the Gerchberg-Saxton algorithm to provide an optimal shaped laser pulse for selective coherent anti-Stokes Raman signal generation of a single component in a mixture.

TOWARDS COHERENT CONTROL OF ENERGETIC MATERIAL INITIATION

We present direct optical initiation (DOI) of energetic materials using coherent control of localized energy deposition. DOI requires depositing energy into the material to produce a critical size hot spot, which allows propagation of the reaction and thereby initiation. The hot spot characteristics needed for growth to initiation can be studied using quantum controlled initiation (QCI). Achieving QCI in condensed phase energetic materials requires optimally shaped ultrafast laser pulses to coherently guide the energy flow along desired paths. As a test of our quantum control capabilities we have successfully demonstrated our ability to control the reaction pathway of the chemical system stilbene. An acousto‐optical modulator based pulse shaper was used at 266 nm, in a shaped pump/supercontinuum probe technique, to enhance and suppress the relative yields of the cis‐ to trans‐stilbene isomerization. The quantum control techniques tested in the stilbene experiments are currently being used to investigate Q...

(U) Implementation and demonstration of a time-resolved pyrometry/spectroscopy capability in shock compression experiments on metal oxide powders

Temperature is notably the most difficult quantity to measure in shock compression experiments; however, it is critical for accurately constraining theoretical or tabular equations of state. Until now, the temperature achieved during the shock loading of porous materials could only be calculated. The technique presented in this report measures, for the first time, the shocked temperature of porous systems.