Direct imaging of ultrafast lattice dynamics

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Presentation transcript:

Direct imaging of ultrafast lattice dynamics by S. Brennan Brown, A. E. Gleason, E. Galtier, A. Higginbotham, B. Arnold, A. Fry, E. Granados, A. Hashim, C. G. Schroer, A. Schropp, F. Seiboth, F. Tavella, Z. Xing, W. Mao, H. J. Lee, and B. Nagler Science Volume 5(3):eaau8044 March 8, 2019 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 1 Experimental configuration of optical drive laser and probe x-ray free-electron laser. Experimental configuration of optical drive laser and probe x-ray free-electron laser. X-ray diffraction captured the lattice response of shocked silicon, showing dynamics of high-pressure phases and melt. X-ray phase-contrast imaging provided direct snapshots of shock propagation in the target and revealed elastic features. These simultaneous, ultrafast measurements allowed resolution of silicon crystalline phases, compression, and density before and after multiple shock features. Upper inset: Unshocked target construction with the shock direction (direction of applied stress) perpendicular (transverse) to the imaging x-ray axis. FLI, Finger Lakes Instrumentation; FEL, free-electron laser. S. Brennan Brown et al. Sci Adv 2019;5:eaau8044 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 2 X-ray data taken at a 15-ns time delay. X-ray data taken at a 15-ns time delay. (A) Phase-contrast images of the 200-μm field-of-view “whole shock” and 10-μm field-of-view spatial scan, revealing a multiple-shockwave structure. On the basis of x-ray diffraction, the first two features (positions 1 and 2) remain in the ambient cubic diamond phase, the third feature is in an inelastic phase transition (position 3), and the sample shows evidence of melt further to the right (positions 4 and 5). Spatial probe placement is accurate within 5 μm. Spatial probes (10-μm field of view) are taken at the following positions from the laser-incident edge of the silicon [100] target in the direction of applied stress: position 1, 125 μm; position 2, 105 μm; position 3, 75 μm; position 4, 62 μm; position 5, 50 μm. (B) Azimuthally integrated x-ray diffraction from a 200-μm x-ray field-of-view (FOV) shot of whole shock and five 10-μm x-ray field-of-view spatial scan shots. Colored lines denote expected locations of silicon high-pressure peaks for relevant phases. Traces are offset to facilitate viewing, but intensity values remain unaltered. S. Brennan Brown et al. Sci Adv 2019;5:eaau8044 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 3 Phase-contrast imaging. Phase-contrast imaging. (A) Intensity lineouts from the phase-contrast imaging data and a forward simulation of phase changes observed across the elastic features. The discrepancy between simulated and observed intensity values at spatial location 135 μm into the target likely emerges as the simulation does not assume any specific shock width or gradient between the two elastic features. (B) Intensity lineouts from imaging at increasing time delays between shock incidence and probe x-ray. An inset graphs the calculated compressions across each elastic feature at increasing time delays. Compression values are only shown for 6-, 8-, and 10-ns delays as the secondary elastic feature only becomes visible at 4 ns. S. Brennan Brown et al. Sci Adv 2019;5:eaau8044 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 4 Shockwave characterization. Shockwave characterization. The bottom image maps the silicon [100] shockwave structure spatially, and black lines mark the densities calculated via phase-contrast imaging and x-ray diffraction. The calculated compression of 14% across E1 takes the unshocked silicon density of 2.33 to 2.65 g/cm3. As the density slope between E1 and E2 is not known, gray dashed lines show the range of potential density values. X-ray diffraction shows evidence of several high-pressure phases of silicon; their densities are mapped in an increasing order. As the sample melts, diffuse scatter overwhelms the x-ray diffraction signal. Silicon structures are reproduced using VESTA (38–40). S. Brennan Brown et al. Sci Adv 2019;5:eaau8044 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 5 Relation between visibility and phase. Relation between visibility and phase. This visibility corresponds to a change in phase induced in the propagated electromagnetic wave as it passes through a density discontinuity in the material. The red dashed line shows the maximum visibility. S. Brennan Brown et al. Sci Adv 2019;5:eaau8044 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).