- Open Access
Imaging of dynamic processes in materials with a laser-wakefield accelerator
Phys. Rev. Applied 24, 064013 – Published 3 December, 2025
DOI: https://doi.org/10.1103/jzzn-bsy8
Abstract
Betatron x rays generated from laser-wakefield accelerators are a promising source for imaging dynamic processes in materials. Here, we present proof-of-concept imaging of microstructural evolution in a hypermonotectic - alloy, which consists of liquid particles in a solid matrix. The images capture the elongation and fragmentation of particles upon isothermal annealing. Because of the femtosecond time scale of the betatron source, the images are not subject to motion blur, whereas the accessibility of the source allows for studies of long-term processes such as annealing. The high-resolution data reveal that the evolution of particles is mediated by an interplay of grain-boundary wetting and morphological instability, in stark contrast to an earlier proposal for (inverse) coarsening.
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References (68)
- R. Cunningham, C. Zhao, N. Parab, C. Kantzos, J. Pauza, K. Fezzaa, T. Sun, and A. D. Rollett, Keyhole threshold and morphology in laser melting revealed by ultrahigh-speed x-ray imaging, Science 363, 849 (2019).
- C. Zhao, N. D. Parab, X. Li, K. Fezzaa, W. Tan, A. D. Rollett, and T. Sun, Critical instability at moving keyhole tip generates porosity in laser melting, Science 370, 1080 (2020).
- L. Zhang, M. Sun, Q. Lv, C. F. Ukaomah, Q. Hu, B. Yu, J. Zhang, X. Liang, G. Wang, and S. Jiang, Evolution of shale microstructure under in situ heat treatment: Synchrotron small-angle X-ray scattering, Energy Fuels 35, 4345 (2021).
- W. L. Tan, N. M. Kirby, Y.-B. Cheng, and C. R. McNeill, Origin of vertical slab orientation in blade-coated layered hybrid perovskite films revealed with in-situ synchrotron X-ray scattering, Nano Energy 83, 105818 (2021).
- M. J. Higgins, J. Kang, G. Huang, D. Montiel, N. Lu, H. Liu, Y.-F. Shen, P. Staublin, J.-S. Park, J. D. Almer, P. Kenesei, P. G. Sanders, R. M. Suter, K. Thornton, and A. J. Shahani, Anomalous strain-energy-driven macroscale translation of grains during nonisothermal annealing, Phys. Rev. Mater. 5, L070401 (2021).
- N. Lu, S. Moniri, M. R. Wiltse, J. Spielman, N. Senabulya, and A. J. Shahani, Dynamics of penetration in textured polycrystal revealed through multimodal three-dimensional analysis, Acta. Mater 217, 117145 (2021).
- X. Wu, H. Liu, and A. Yan, Phase-contrast X-ray tomography: Contrast mechanism and roles of phase retrieval, Eur. J. Radiol. 68, S8 (2008).
- P. Cloetens, R. Barrett, J. Baruchel, J.-P. Guigay, and M. Schlenker, Phase objects in synchrotron radiation hard x-ray imaging, J. Phys. D: Appl. Phys. 29, 133 (1996).
- A. Bhattacharya, Y.-F. Shen, C. M. Hefferan, S. F. Li, J. Lind, R. M. Suter, C. E. Krill, and G. S. Rohrer, Grain boundary velocity and curvature are not correlated in polycrystals, Science 374, 189 (2021).
- Z. Xu, Y.-F. Shen, S. K. Naghibzadeh, X. Peng, V. Muralikrishnan, S. Maddali, D. Menasche, A. R. Krause, K. Dayal, R. M. Suter, and G. S. Rohrer, Grain boundary migration in polycrystalline -, Acta Mater. 264, 119541 (2024).
- Z. Ren, L. Gao, S. J. Clark, K. Fezzaa, P. Shevchenko, A. Choi, W. Everhart, A. D. Rollett, L. Chen, and T. Sun, Machine learning–aided real-time detection of keyhole pore generation in laser powder bed fusion, Science 379, 89 (2023).
- X. Lei, Y. Zhang, J. Sun, F. Bachmann, X. Yang, R. E. Sanders, and D. Juul Jensen, Particle stimulated nucleation revisited in three dimensions: A laboratory-based multimodal X-ray tomography investigation, Mater. Res. Lett. 9, 65 (2021).
- J. R. Schneider, R. Bouchard, T. Brückel, M. Lippert, H.-B. Neumann, H. F. Poulsen, U. Rütt, T. Schmidt, and M. von Zirnmermann, High energy synchrotron radiation. A new probe for condensed matter research, J. Phys. IV 04, C9 (1994).
- B. Günther, R. Gradl, C. Jud, E. Eggl, J. Huang, S. Kulpe, K. Achterhold, B. Gleich, M. Dierolf, and F. Pfeiffer, The versatile X-ray beamline of the Munich Compact Light Source: Design, instrumentation and applications, J. Synchrotron Radiat. 27, 1395 (2020).
- A. E. Hussein et al., Laser-wakefield accelerators for high-resolution X-ray imaging of complex microstructures, Sci. Rep. 9, 3249 (2019).
- N. Lu, J. Kang, N. Senabulya, R. Keinan, N. Gueninchault, and A. J. Shahani, Dynamics of particle-assisted abnormal grain growth revealed through integrated three-dimensional microanalysis, Acta Mater. 195, 1 (2020).
- D. H. Larsson, W. Vågberg, A. Yaroshenko, A. Ö. Yildirim, and H. M. Hertz, High-resolution short-exposure small-animal laboratory x-ray phase-contrast tomography, Sci. Rep. 6, 39074 (2016).
- P. Bidola, K. Morgan, M. Willner, A. Fehringer, S. Allner, F. Prade, F. Pfeiffer, and K. Achterhold, Application of sensitive, high-resolution imaging at a commercial lab-based X-ray micro-CT system using propagation-based phase retrieval, J. Microsc. 266, 211 (2017).
- N. Arai, T. Stan, S. Macfarland, P. W. Voorhees, N. S. Muyanja, A. J. Shahani, and K. T. Faber, Coarsening of dendrites in solution-based freeze-cast ceramic systems, Acta Mater. 215, 117039 (2021).
- V. M. Segal, Materials processing by simple shear, Mater. Sci. Eng.: A 197, 157 (1995).
- J. M. Cole et al., High-resolution of a mouse embryo using a compact laser-driven X-ray betatron source, Proc. Natl. Acad. Sci. 115, 6335 (2018).
- R. C. Shah, F. Albert, K. Ta Phuoc, O. Shevchenko, D. Boschetto, A. Pukhov, S. Kiselev, F. Burgy, J.-P. Rousseau, and A. Rousse, Coherence-based transverse measurement of synchrotron x-ray radiation from relativistic laser-plasma interaction and laser-accelerated electrons, Phys. Rev. E 74, 045401(R) (2006).
- S. Kneip et al., Bright spatially coherent synchrotron X-rays from a table-top source, Nat. Phys. 6, 980 (2010).
- S. Kneip, C. McGuffey, F. Dollar, M. S. Bloom, V. Chvykov, G. Kalintchenko, K. Krushelnick, A. Maksimchuk, S. P. Mangles, T. Matsuoka, Z. Najmudin, C. A. Palmer, J. Schreiber, W. Schumaker, A. G. Thomas, and V. Yanovsky, X-ray phase contrast imaging of biological specimens with femtosecond pulses of betatron radiation from a compact laser plasma wakefield accelerator, Appl. Phys. Lett. 99, 093701 (2011).
- M. Kozlova, I. Andriyash, J. Gautier, S. Sebban, S. Smartsev, N. Jourdain, U. Chaulagain, Y. Azamoum, A. Tafzi, J. P. Goddet, K. Oubrerie, C. Thaury, A. Rousse, and K. Ta Phuoc, Hard x rays from laser-wakefield accelerators in density tailored plasmas, Phys. Rev. X 10, 011061 (2020).
- R. Rakowski, P. Zhang, K. Jensen, B. Kettle, T. Kawamoto, S. Banerjee, C. Fruhling, G. Golovin, D. Haden, M. S. Robinson, D. Umstadter, B. A. Shadwick, and M. Fuchs, Transverse oscillating bubble enhanced laser-driven betatron X-ray radiation generation, Sci. Rep. 12, 10855 (2022).
- S. Fourmaux, E. Hallin, U. Chaulagain, S. Weber, and J. C. Kieffer, Laser-based synchrotron X-ray radiation experimental scaling, Opt. Express 28, 3147 (2020).
- H. Zhang et al., High-brightness betatron X-ray source driven by the SULF-1 PW laser, High Power Laser Sci. Eng. 13, e31 (2025).
- F. Albert and A. G. R. Thomas, Applications of laser wakefield accelerator-based light sources, Plasma Phys. Controlled Fusion 58, 103001 (2016).
- V. Senthilkumaran, N. F. Beier, S. Fourmaux, P. Shabaninezhad, J. Stinehart, L. Zhou, J. A. Moore, and A. E. Hussein, Laser-driven betatron x rays for high-throughput imaging of additively manufactured materials, Rev. Sci. Instrum. 95, 123510 (2024).
- A. E. Bravo, H. A. Durán, V. H. Jacobo, A. Ortiz, and R. Schouwenaars, Towards new formulations for journal bearing alloys, Wear 302, 1528 (2013).
- Z.-M. Wang, Q. Yang, Z.-P. Sun, B.-R. Zhang, W. Zhao, and W.-F. Rao, The effects of and on the soft phase in sliding bearing alloy, Mater. Charact. 170, 110684 (2020).
- L. Ratke and S. Diefenbach, Liquid immiscible alloys, Mater. Sci. Eng.: R: Rep. 15, 263 (1995).
- K. Lepper, M. James, J. Chashechkina, and D. A. Rigney, Sliding behavior of selected aluminum alloys, Wear 203–204, 46 (1997).
- B. Prinz, A. Romero, and L. Ratke, Casting process for hypermonotectic alloys under terrestrial conditions, J. Mater. Sci. 30, 4715 (1995).
- M. Zha, Z.-Y. Yu, F. Qian, H.-Y. Wang, Y.-J. Li, R. H. Mathiesen, and H. J. Roven, Achieving dispersed fine soft particles and grain refinement in a hypermonotectic – alloy by severe plastic deformation and annealing, Scr. Mater. 155, 124 (2018).
- J. M. García-Infanta, S. Swaminathan, A. P. Zhilyaev, F. Carreño, O. A. Ruano, and T. R. McNelley, Microstructural development during equal channel angular pressing of hypo-eutectic – casting alloy by different processing routes, Mater. Sci. Eng.: A 485, 160 (2008).
- C. H. Su and P. W. Voorhees, The dynamics of precipitate evolution in elastically stressed solids—I. Inverse coarsening, Acta Mater. 44, 1987 (1996).
- R. J. Shalloo et al., Automation and control of laser wakefield accelerators using Bayesian optimization, Nat. Commun. 11, 6355 (2020).
- P. Modregger, D. Lübbert, P. Schäfer, and R. Köhler, Spatial resolution in Bragg-magnified X-ray images as determined by Fourier analysis, Phys. Status Solidi A 204, 2746 (2007).
- S. Corde, K. Ta Phuoc, G. Lambert, R. Fitour, V. Malka, A. Rousse, A. Beck, and E. Lefebvre, Femtosecond x rays from laser-plasma accelerators, Rev. Mod. Phys. 85, 1 (2013).
- P. Willmott, in An Introduction to Synchrotron Radiation (John Wiley & Sons, Hoboken, New Jersey, USA, 2019), Chap. 8, pp. 367–402.
- Synchrotron Radiation: Basics, Methods and Applications, edited by S. Mobilio, F. Boscherini, and C. Meneghini (Springer, Berlin, Heidelberg, 2015).
- H. W. Kuhn, The Hungarian method for the assignment problem, Nav. Res. Logist. Q. 2, 83 (1955).
- J. Munkres, Algorithms for the assignment and transportation problems, J. Soc. Ind. Appl. Math. 5, 32 (1957).
- K. Riesen and H. Bunke, Approximate graph edit distance computation by means of bipartite graph matching, Image Vis. Comput. 27, 950 (2009).
- R. Balluffi, S. Allen, and W. Carter, in Kinetics of Materials (John Wiley & Sons, Hoboken, New Jersey, USA, 2005), pp. 335–336.
- P. W. Voorhees, The theory of Ostwald ripening, J. Stat. Phys. 38, 231 (1985).
- In the quasi-steady state, the critical size is of the same order of magnitude as the mean particle size (minor-axis length), ; according to the data presented in Fig. 2, .
- H. J. Vogel and L. Ratke, Instability of grain boundary grooves due to equilibrium grain boundary diffusion, Acta Metall. Mater. 39, 641 (1991).
- B. B. Straumal, W. Gust, and D. A. Molodov, Wetting transition on grain boundaries in contacting with a -rich melt, Interface Sci. 3, 127 (1995).
- B. Straumal, T. Muschik, W. Gust, and B. Predel, The wetting transition in high and low energy grain boundaries in the () system, Acta Metall. Mater. 40, 939 (1992).
- R. C. Hugo and R. G. Hoagland, In-situ TEM observation of aluminum embrittlement by liquid gallium, Scr. Mater. 38, 523 (1998).
- E. E. Glickman and M. Nathan, On the kinetic mechanism of grain boundary wetting in metals, J. Appl. Phys. 85, 3185 (1999).
- B. Straumal, E. Rabkin, W. Łojkowski, W. Gust, and L. S. Shvindlerman, Pressure influence on the grain boundary wetting phase transition in alloys, Acta Mater. 45, 1931 (1997).
- The critical wavelength can be determined by finding the point of intersection between the curves (Fig. 3) and , where is the major-axis length of the particle (not pictured). Note that and are related under the assumption that the particle volume is conserved [see also Eq. (G2)].
- W. Gust, S. Mayer, A. Bögel, and B. Predel, Generalized representation of grain boundary self-diffusion data, J. Phys. Colloq. 46, C4 (1985).
- G. Gottstein, D. Molodov, and L. Shvindlerman, in Metals Process Simulation (ASM International, Materials Park, Ohio, USA, 2010).
- D. Guénot, D. Gustas, A. Vernier, B. Beaurepaire, F. Böhle, M. Bocoum, M. Lozano, A. Jullien, R. Lopez-Martens, A. Lifschitz, and J. Faure, Relativistic electron beams driven by kHz single-cycle light pulses, Nat. Photonics 11, 293 (2017).
- C. N. Danson et al., Petawatt and exawatt class lasers worldwide, High Power Laser Sci. Eng. 7, e54 (2019/ed).
- The data are available at https://doi.org/10.5281/zenodo.17359670.
- V. V. Stolyarov, Y. T. Zhu, I. V. Alexandrov, T. C. Lowe, and R. Z. Valiev, Influence of ECAP routes on the microstructure and properties of pure , Mater. Sci. Eng.: A 299, 59 (2001).
- P. Perona and J. Malik, Scale-space and edge detection using anisotropic diffusion, IEEE Trans. Pattern Anal. Mach. Intell. 12, 629 (1990).
- F. Bachmann, R. Hielscher, and H. Schaeben, Texture analysis with MTEX—Free and open source software toolbox, Solid State Phenom. 160, 63 (2010).
- A. M. Brown and M. F. Ashby, Correlations for diffusion constants, Acta Metall. 28, 1085 (1980).
- T. Uesugi and K. Higashi, First-principles calculation of grain boundary energy and grain boundary excess free volume in aluminum: Role of grain boundary elastic energy, J. Mater. Sci. 46, 4199 (2011).
- C. B. Porth and J. R. Cahoon, Interdiffusion of in liquid , J. Phase Equilib. Diffus. 31, 149 (2010).
- Thermo-Calc Software TCAL6 -alloys database version 6.0.