- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Letters

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Broadband Ptychotomography with a Hyperspectral Detector

Wiebe Stolp1,*, Frederic van Assche1, Ruizhi Tang1, Karel Desplenter1, Caori Organista Castelblanco1, Ralf Ziesche2, Silvia Cipiccia3, Darren Batey4, and Matthieu N. Boone1,†

  • *Contact author: wiebestolp@gmail.com
  • †Contact author: matthieu.boone@ugent.be
PDF

Phys. Rev. Lett. 134, 257001 – Published 27 June, 2025

DOI: https://doi.org/10.1103/kbrf-gb9c

Abstract

X-ray ptychography is a robust microscopy technique with nanoscale resolution that requires a spatially and temporally coherent illumination. In a typical setup, the temporal coherence requirements are satisfied by monochromating the x-ray source, e.g., using a crystal monochromator. Recent studies have shown that energy resolving, or hyperspectral, detectors can to some extent replace the role of the monochromator to perform, e.g., edge-subtraction ptychographic imaging with broadband radiation in a single acquisition. Scaling this capability from two dimensions (2D) to three dimensions (3D), and from a single absorption edge to multiple edges, is critical for its applications in structural and elemental characterisation. The method is hitherto limited by the inherently lower maximum count rate of hyperspectral detectors and the chromaticity of the optics often used in x-ray ptychography experiments, namely Fresnel zone plates. In this work, we design an optimized broadband spectroscopic ptychography setup and use it to perform 3D hyperspectral imaging of particles of battery material containing various percentages of nickel, manganese, cobalt (NMC). We show that we can identify different compositions based on their spectral response. We discuss the results and provide guidelines for future exploitation of the method in laboratory settings.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (41)

  1. J. M. Rodenburg, A. C. Hurst, A. G. Cullis, B. R. Dobson, F. Pfeiffer, O. Bunk, C. David, K. Jefimovs, and I. Johnson, Hard-x-ray lensless imaging of extended objects, Phys. Rev. Lett. 98, 034801 (2007).
  2. F. Pfeiffer, X-ray ptychography, Nat. Photonics 12, 9 (2018).
  3. J. Miao, R. L. Sandberg, and C. Song, Coherent x-ray diffraction imaging, IEEE J. Sel. Top. Quantum Electron. 18, 399 (2012).
  4. T. Aidukas, N. W. Phillips, A. Diaz, E. Poghosyan, E. Müller, A. F. J. Levi, G. Aeppli, M. Guizar-Sicairos, and M. Holler, High-performance 4-nm-resolution x-ray tomography using burst ptychography, Nature (London) 632, 81 (2024).
  5. D. J. Batey, S. Cipiccia, F. Van Assche, S. Vanheule, J. Vanmechelen, M. N. Boone, and C. Rau, Spectroscopic imaging with single acquisition ptychography and a hyperspectral detector, Sci. Rep. 9, 12278 (2019).
  6. A. M. Wise, J. N. Weker, S. Kalirai, M. Farmand, D. A. Shapiro, F. Meirer, and B. M. Weckhuysen, Nanoscale chemical imaging of an individual catalyst particle with soft x-ray ptychography, ACS Catal. 6, 2178 (2016).
  7. F. Bardelli, F. Brun, S. De Panfilis, P. Cloetens, S. Capella, E. Belluso, D. Bellis, A. Di Napoli, and A. Cedola, Chemo-physical properties of asbestos bodies in human lung tissues studied at the nano-scale by non-invasive, Toxicol. Lett. 348, 18 (2021).
  8. D. J. Batey, T. B. Edo, C. Rau, U. Wagner, Z. D. Pešić, T. A. Waigh, and J. M. Rodenburg, Reciprocal-space up-sampling from real-space oversampling in x-ray ptychography, Phys. Rev. A 89, 043812 (2014).
  9. W. Stolp, S. Cipiccia, D. Batey, and M. N. Boone, Optics for broadband x-ray ptychography (to be published).
  10. L. Loetgering, X. Liu, A. C. C. D. Beurs, M. Du, G. Kuijper, K. S. E. Eikema, and S. Witte, Tailoring spatial entropy in extreme ultraviolet focused beams for multispectral ptychography, Optica 8, 130 (2021).
  11. D. Batey, S. Cipiccia, X. Shi, S. Williams, K. Wanelik, A. Wilson, S. Pérez-Tamarit, P. Cimavilla, M. A. Ródriguez-Pérez, and C. Rau, Coherence branch at I13, DLS: The multiscale, multimodal, ptycho-tomographic end station, Microsc. Microanal. 24, 40 (2018).
  12. D. A. Mossessian and P. A. Heimann, Characterization of ALS undulator radiation—high K, taper, and the near field effect, Rev. Sci. Instrum. 66, 5153 (1995).
  13. I. Ordavo et al., A new pnCCD-based color x-ray camera for fast spatial and energy-resolved measurements, Nucl. Instrum. Methods Phys. Res., Sect. A 654, 250 (2011).
  14. A. Bjeoumikhov, G. Buzanich, N. Langhoff, I. Ordavo, M. Radtke, U. Reinholz, H. Riesemeier, O. Scharf, H. Soltau, and R. Wedell, The SLcam: A full-field energy dispersive x-ray camera, J. Instrum. 7, C11008 (2012).
  15. G. F. Knoll, Radiation Detection and Measurement (John Wiley & Sons, New York, 2010).
  16. M. N. Boone, J. Garrevoet, P. Tack, O. Scharf, D. P. Cormode, D. Van Loo, E. Pauwels, M. Dierick, L. Vincze, and L. Van Hoorebeke, High spectral and spatial resolution x-ray transmission radiography and tomography using a Color X-ray Camera, Nucl. Instrum. Methods Phys. Res., Sect. A 735, 644 (2014).
  17. F. Van Assche, S. Vanheule, L. Van Hoorebeke, and M. N. Boone, The spectral x-ray imaging data acquisition (SpeXIDAQ) framework, Sensors (Switzerland) 21, 563 (2021).
  18. T. M. M. Heenan, A. Wade, C. Tan, J. E. Parker, D. Matras, A. S. Leach, J. B. Robinson, A. Llewellyn, A. Dimitrijevic, R. Jervis, P. D. Quinn, D. J. L. Brett, and P. R. Shearing, Identifying the origins of microstructural defects such as cracking within Ni-Rich NMC811 cathode particles for lithium-ion batteries, Adv. Energy Mater. 10, 2002655 (2020).
  19. T. M. M. Heenan, A. V. Llewellyn, A. S. Leach, M. D. R. Kok, C. Tan, R. Jervis, D. J. L. Brett, and P. R. Shearing, Resolving Li-ion battery electrode particles using rapid lab-based x-ray nano-computed tomography for high-throughput quantification, Adv. Sci. 7, 2000362 (2020).
  20. C. Zhan, T. Wu, J. Lu, and K. Amine, Dissolution, migration, and deposition of transition metal ions in Li-ion batteries exemplified by Mn-based cathodes—a critical review, Energy Environ. Sci. 11, 243 (2018).
  21. L. R. Brandt, J.-J. Marie, T. Moxham, D. P. Förstermann, E. Salvati, C. Besnard, C. Papadaki, Z. Wang, P. G. Bruce, and A. M. Korsunsky, Synchrotron x-ray quantitative evaluation of transient deformation and damage phenomena in a single nickel-rich cathode particle, Energy Environ. Sci. 13, 3556 (2020).
  22. See Supplemental Material at http://link.aps.org/supplemental/10.1103/kbrf-gb9c for a video of the 3D rendering, ptychographic reconstructions across the whole energy range, and a full absorption spectrum of the different particles.
  23. D. Batey, Ptychographic imaging of mixed states, Ph.D. thesis, University of Scheffield, 2014.
  24. A. M. Maiden and J. M. Rodenburg, An improved ptychographical phase retrieval algorithm for diffractive imaging, Ultramicroscopy 109, 1256 (2009).
  25. D. Gürsoy, Y. P. Hong, K. He, K. Hujsak, S. Yoo, S. Chen, Y. Li, M. Ge, L. M. Miller, Y. S. Chu, V. De Andrade, K. He, O. Cossairt, A. K. Katsaggelos, and C. Jacobsen, Rapid alignment of nanotomography data using joint iterative reconstruction and reprojection, Sci. Rep. 7, 11818 (2017).
  26. D. Gürsoy, F. De Carlo, X. Xiao, and C. Jacobsen, TomoPy: A framework for the analysis of synchrotron tomographic data, J. Synchrotron Radiat. 21, 1188 (2014).
  27. P. Gilbert, Iterative methods for the three-dimensional reconstruction of an object from projections, J. Theor. Biol. 36, 105 (1972).
  28. D. H. Bailey and P. N. Swarztrauber, The fractional Fourier transform and applications, SIAM Rev. 33, 389 (1991).
  29. M. Guizar-Sicairos, S. T. Thurman, and J. R. Fienup, Efficient subpixel image registration algorithms, Opt. Lett. 33, 156 (2008).
  30. D. H. Larsson, P. a. C. Takman, U. Lundström, A. Burvall, and H. M. Hertz, A 24 keV liquid-metal-jet x-ray source for biomedical applications, Rev. Sci. Instrum. 82, 123701 (2011).
  31. D. J. Batey, F. Van Assche, S. Vanheule, M. N. Boone, A. J. Parnell, O. O. Mykhaylyk, C. Rau, and S. Cipiccia, X-ray ptychography with a laboratory source, Phys. Rev. Lett. 126, 193902 (2021).
  32. P. Zhang, J. Zhao, B. Lin, X. Wu, and G. Cui, Hyperspectral microscopy imaging based on Fourier ptychographic microscopy, J. Opt. 24, 055301 (2022).
  33. B. Zhang, D. F. Gardner, M. H. Seaberg, E. R. Shanblatt, C. L. Porter, R. Karl, C. A. Mancuso, H. C. Kapteyn, M. M. Murnane, and D. E. Adams, Ptychographic hyperspectral spectromicroscopy with an extreme ultraviolet high harmonic comb, Opt. Express 24, 18745 (2016).
  34. L. Loetgering, S. Witte, and J. Rothhardt, Advances in laboratory-scale ptychography using high harmonic sources [Invited], Opt. Express 30, 4133 (2022).
  35. D. J. Batey, D. Claus, and J. M. Rodenburg, Information multiplexing in ptychography, Ultramicroscopy 138, 13 (2014).
  36. L. Jones, S. Bell, B. Cline, T. Gardiner, M. Hart, M. Prydderch, P. Seller, M. Veale, and M. Wilson, Spectroscopic x-ray imaging at MHz frame rates—the HEXITECMHz ASIC, J. Instrum. 17, C10012 (2022).
  37. A. Bergamaschi et al., The MÖNCH detector for soft x-ray, high-resolution, and energy resolved applications, Synchrotron Radiat. News 31, 11 (2018).
  38. B. L. Henke, E. M. Gullikson, and J. C. Davis, X-ray interactions: Photoabsorption, scattering, transmission, and reflection at E=50–30,000  eV, Z=1–92, At. Data Nucl. Data Tables 54, 181 (1993).
  39. J. Spence, U. Weierstall, and M. Howells, Coherence and sampling requirements for diffractive imaging, Ultramicroscopy 101, 149 (2004).
  40. D. Paganin, Coherent X-Ray Optics (Oxford University Press, New York, 2006).
  41. B. Lai, W. B. Yun, D. Legnini, Y. Xiao, J. Chrzas, P. J. Viccaro, V. White, S. Bajikar, D. Denton, F. Cerrina, E. Di Fabrizio, M. Gentili, L. Grella, and M. Baciocchi, Hard x-ray phase zone plate fabricated by lithographic techniques, Appl. Phys. Lett. 61, 1877 (1992).

Outline

Information

Phys. Rev. Lett. 134, 257001– Published 27 June, 2025
  • Received 15 November 2024
  • Accepted 2 May 2025
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation