Real-time synchrotron diffraction has been used to monitor the phase transformations of highly exothermic, fast self-propagating solid combustion reactions on a subsecond time scale down to 100 milliseconds and in some instances to 10 milliseconds. Three systems were investigated: Ti + C --> TiC; Ti + C + xNi --> TiC + Ni-Ti alloy; and Al + Ni --> AlNi. In all three reactions, the first step was the melting of the metal reactants. Formation of TiC in the first two reactions was completed within 400 milliseconds of the melting of the Ti metal, indicating that the formation of TiC took place during the passage of the combustion wave front. In the Al + Ni reaction, however, passage of the wave front was followed by the appearance and disappearance of at least one intermediate in the afterburn region. The final AlNi was formed some 5 seconds later and exhibited a delayed appearance of the (210) reflection, which tends to support a phase transformation from a disordered AlNi phase at high temperature to an ordered CsCl structure some 20 seconds later. This new experimental approach can be used to study the chemical dynamics of high-temperature solid-state phenomena and to provide the needed database to test various models for solid combustion.
The formation of TaC and Ta2C by combustion synthesis from their elemental constituents has been studied by time-resolved x-ray diffraction (TRXRD) using synchrotron radiation. The reactions have been followed with a time resolution down to 50 ms. Since the adiabatic temperatures for both reactions are well below any liquidus temperature in the Ta—C phase diagram, no melting occurs and these combustion reactions occur purely in the solid state. The phase transformations associated with these reactions are followed by monitoring the disappearance of reactant and appearance of product powder diffraction peaks in real time as the reaction front propagates through the combusting specimen. In the synthesis of TaC, the results show the formation of the subcarbide (Ta2C phase as an intermediate. In the synthesis of Ta2C, the reaction proceeds directly to the product with no discernible intermediate Ta–C phase within a 50 ms time frame. The chemical dynamics associated with the combustion synthesis of TaC may be described by an initial phase transformation to hexagonal Ta2C arising from carbon diffusion into the Ta metal lattice. As more carbon is available this intermediate subcarbide phase, which has one-half of its octahedral interstices occupied by the carbon, further transforms to the cubic TaC final product, in which all octahedral sites are now occupied. The time-resolved data indicate that the rate of formation of Ta2C is a factor of two faster than that of TaC.
The Dante soft x-ray spectrometer, installed on the Omega laser facility at the Laboratory for Laser Energetics, University of Rochester, is a 12-channel filter-edge defined soft x-ray power diagnostic. It is used to measure the spectrally resolved, absolute flux from direct drive, indirect drive (hohlraums) and other plasma sources. Dante component calibration efforts using two beam lines, U3C (50 eV-1 keV) and X8A (1-6 keV) at the National Synchrotron Light Source have been implemented to improve the accuracy of these measurements. We have calibrated metallic vacuum x-ray diodes, mirrors and filters.
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