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Title: X-ray diffraction studies of shock compressed bismuth using X-ray free electron lasers
Author: Gorman, Martin Gerard
ISNI:       0000 0004 6499 9861
Awarding Body: University of Edinburgh
Current Institution: University of Edinburgh
Date of Award: 2016
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The ability to diagnose the structure of a material at extreme conditions of high-pressure and high-temperature is fundamental to understanding its behaviour, especially since it was found that materials will adopt complex crystal structures at pressures in the Terapascal regime (1TPa). Static compression, using the diamond anvil cell coupled with synchrotron radiation has to date been the primary method for structural studies of materials at high pressure. However, dynamic compression is the only method capable of reaching pressures comparable to the conditions found in the interior of newly discovered exo-planets and gas giants where such exotic high-pressure behaviour is predicted to be commonplace among materials. While generating extreme conditions using shock compression has become a mature science, it has proved a considerable experimental challenge to directly observe and study such phase transformations that have been observed using static studies due to the lack of sufficiently bright X-ray sources. However, the commissioning of new 4th generation light sources known as free electron lasers now provide stable, ultrafast pulses of X-rays of unprecedented brightness allowing in situ structural studies of shock compressed materials and their phase transformation kinetics in unprecedented detail. Bismuth, with its highly complex phase diagram at modest pressures and temperatures, has been one of the most studied systems using both static and dynamic compression. Despite this, there has been no structural characterisation of the phases observed on shock compression and it is therefore the ideal candidate for the first structural studies using X-ray radiation from a free electron laser. Here, bismuth was shock compressed with an optical laser and probed in situ with X-ray radiation from a free electron laser. The evolution of the crystal structure (or lack there of) during compression and shock release are documented by taking snapshots of successive experiments, delayed in time. The melting of Bi on release from Bi-V was studied, with precise time scans showing the pressure releasing from high-pressure Bi-V phase until the melt curve is reached off-Hugoniot. Remarkable agreement with the equilibrium melt curve is found and the promise of this technique has for future off-Hugoniot melt curve studies at extreme conditions is discussed. In addition, shock melting studies of Bi were performed. The high-pressure Bi - V phase is observed to melt along the Hugoniot where melting is unambiguously identified with the emergence of a broad liquid-scattering signature. These measurements definitively pin down where the Hugoniot intersects the melt curve - a source of some disagreement in recent years. Evidence is also presented for a change in the local structure of the liquid on shock release. The impact of these results are discussed. Finally, a sequence of solid-solid phase transformations is observed on shock compression as well as shock release and is detected by distinct changes in the obtained diffraction patterns. The well established sequence of solid-solid phase transformations observed in previous static studies is not observed in our experiments. Rather, Bi is found to exist in some metastable structures instead of forming equilibrium phases. The implications these results have for observing reconstructive phase transformations in other materials on shock timescales are discussed.
Supervisor: McMahon, Malcolm ; Loveday, John Sponsor: Engineering and Physical Sciences Research Council (EPSRC)
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: bismuth ; shock compression ; X-ray diffraction ; free electron laser