arXiv subjects

Hoelen L. Lalandec Robert

Publications and source records attributed to Hoelen L. Lalandec Robert.

8 recordsLinked to original sources

arXiv2026

Interactive event-driven 4D-STEM with Timepix4 and live analytical ptychography

Four-dimensional scanning transmission electron microscopy provides access to rich diffraction information at every probe position, but the high data rates associated with pixelated detectors remain a major challenge for interactive operation. Event-driven detectors offer an efficient alternative by representing the measurement as a sparse stream of individual incidences, substantially reducing requirements related to data handling and enabling on-the-fly processing. Here, we develop a high-throughput, real-time, 4D-STEM workflow based on the Timepix4 detector and demonstrate its operation at microsecond dwell times and standard beam currents. A common clock shared by the scan unit and detector allows the probe position of each electron event to be determined directly from its time-of-arrival, eliminating the need for inter-stream synchronization and enabling fully concurrent and independent multi-stream processing. The resulting pipeline continuously processes the detector data during acquisition, with the reconstructed images directly available. We demonstrate live virtual annular detector imaging, Real-Time Integration Center of Mass and direct electron ptychography within the guided progressive reconstructive imaging framework. The workflow sustains the high event rates of Timepix4 while maintaining zero latency for live interactive operation, thus extending event-driven 4D-STEM towards beam currents and acquisition conditions beyond those previously demonstrated with Timepix3-based systems. These results demonstrate that the combination of high-bandwidth event-driven detection, hardware-level synchronization and parallel processing can transform 4D-STEM from an offline technique into an interactive imaging modality, in which dose-efficient phase contrast and diffraction-based signals can serve directly as immediate feedback during STEM experiments.

physics.ins-det↗

arXiv2026

Pushing the Dose Limit of Atomic-Resolution Imaging: A 4D-STEM case study of NaCl

Beam-induced damage fundamentally limits the characterization of beam-sensitive materials by scanning transmission electron microscopy (STEM), since structural information must be recorded before the electron beam irreversibly modifies the specimen. Here, sodium chloride (NaCl) is employed as a model beam-sensitive ionic crystal to investigate beam-induced structural evolution and the low-dose regime in which useful structural information can be recovered prior to significant damage. Four-dimensional STEM (4D-STEM) datasets were acquired at 200 kV using a Timepix3 direct electron detector and reconstructed using real-time integrated centre of mass (riCoM) imaging. We first establish the characteristic damage behavior of NaCl under high electron doses. Across different dwell times and raster scan orientations, damage develops reproducibly into square-faceted voids whose boundaries align with the 100 crystallographic directions of the rock-salt lattice, indicating that the morphology is governed predominantly by the intrinsic crystallography rather than the scan geometry. We then investigate the low-dose imaging regime using dose-fractionated acquisitions. At 130 e-A-2 per frame, normalized cross-correlation with respect to the first frame quantitatively tracks progressive structural degradation and enables the onset of measurable damage to be identified as a function of accumulated dose. A subsequent acquisition at 32 e-A-2 per frame demonstrates that atomic-scale spatial information can still be recovered below this damage threshold. These results demonstrate how dose-efficient 4D-STEM acquisition combined with riCoM imaging can extend the accessible imaging regime of highly beam-sensitive ionic materials while preserving atomic-scale information.

physics.app-ph↗

arXiv2026

Guided progressive reconstructive imaging: a new quantization-based framework for low-dose, high-throughput and real-time analytical ptychography

By profiting from recent developments in detector technologies, making it possible to access a stream of detection events with few-ns time resolutions, a new ptychographic workflow is established. This methodological framework, referred to as guided progressive reconstructive imaging, relies on a quantization-based description of the acquired intensity, through an elementary derivation. Established direct phase retrieval solutions, such as the Wigner distribution deconvolution approach, can then be adapted to a continuous treatment of received counts, with no need for a dense data representation. Consequently, the result is obtained in the form of a progressively improving estimate, while providing immediate user feedback thanks to a processing speed high enough to surpass the acquisition bandwidth. This fast measurement is enabled by the cumulative usage of a pre-calculated library of kernel-limited functions, accumulating count-wise contributions as a function of the triggered detector pixel. Hence, the reconstruction offers the same advantages of direct phase retrieval methods, in particular a high dose-efficiency and the absence of complex convergence dynamics, with much less stringent restrictions on the field of view than is typical in current alternatives. Its implementation is also significantly more straightforward and flexible. Overall, this work constitutes a major evolution in the state-of-the-art, facilitating repeatable and low-dose experiments with high accessibility, and being applicable to electron-based imaging, X-ray diffraction and optical microscopy.

physics.app-ph↗

arXiv2026

Improving the low-dose performance of aberration correction in single sideband ptychography

The single sideband (SSB) framework of analytical electron ptychography can account for the presence of residual geometrical aberrations induced by the probe-forming lens. However, the accuracy of this aberration correction method is highly sensitive to noise, in part due to the necessity of phase unwrapping. In this work, we thus propose two strategies to improve aberration correction performance in low-dose conditions: confining phase unwrapping within the sidebands and selecting only well-unwrapped sidebands for calculating aberration coefficients. These strategies are validated through SSB reconstructions of both simulated and experimental 4D-STEM datasets of monolayer tungsten diselenide (WSe2). A comparison of results demonstrates significant improvements in Poisson noise tolerance, making aberration correction more robust and reliable for low-dose imaging.

physics.app-ph↗

arXiv2025

Investigating the convergence properties of iterative ptychography for atomic-resolution low-dose imaging

This study investigates the convergence properties of a collection of iterative electron ptychography methods, under low electron doses ($<$ 10$^3$ $e^-/A^2$) and gives particular attention to the impact of the user-defined update strengths. We demonstrate that carefully chosen values for this parameter, ideally smaller than those conventionally met in the literature, are essential for achieving accurate reconstructions of the projected electrostatic potential. Using a 4D dataset of a thin hybrid organic-inorganic formamidinium lead bromide (FAPbBr$_{3}$) sample, we show that convergence is in practice achievable only when the update strengths for both the object and probe are relatively small compared to what is found in literature. Additionally we demonstrate that under low electron doses, the reconstructions initial error increases when the update strength coefficients are reduced below a certain threshold emphasizing the existence of critical values beyond which the algorithms are trapped in local minima. These findings highlight the need for carefully optimized reconstruction parameters in iterative ptychography, especially when working with low electron doses, ensuring both effective convergence and correctness of the result.

cond-mat.mtrl-sci↗

arXiv2025

Removing constraints of 4D-STEM with a framework for event-driven acquisition and processing

Pixelated detectors in scanning transmission electron microscopy (STEM) generate large volumes of data, often tens to hundreds of GB per scan. However, to make current advancements scalable and enable widespread adoption, it is essential to use the most efficient representation of an electron's information. Event-driven direct electron detectors, such as those based on the Timepix3 chip, offer significant potential for electron microscopy, particularly for low-dose experiments and real-time data processing. In this study, we compare sparse and dense data representations in terms of their size and computational requirements across various 4D-STEM scenarios, including high-resolution imaging and nano-beam electron diffraction. The advantages of performing 4D-STEM in an event-driven mode - such as reduced requirements in memory, bandwidth, and computational demands - can only be fully leveraged if the entire acquisition and processing pipeline is optimized to work directly with the event format, avoiding intermediate dense representations. We introduce a framework designed for acquisition and processing based on this event format, and demonstrate live processing of event-driven 4D-STEM, including analytical ptychography.

physics.ins-det↗

arXiv2025

Roadmap for Quantum Nanophotonics with Free Electrons

Over the past century, continuous advancements in electron microscopy have enabled the synthesis, control, and characterization of high-quality free-electron beams. These probes carry an evanescent electromagnetic field that can drive localized excitations and provide high-resolution information on material structures and their optical responses, currently reaching the sub-ångström and few-meV regime. Moreover, combining free electrons with pulsed light sources in ultrafast electron microscopy adds temporal resolution in the sub-femtosecond range while offering enhanced control of the electron wave function. Beyond their exceptional capabilities for time-resolved spectromicroscopy, free electrons are emerging as powerful tools in quantum nanophotonics, on par with photons in their ability to carry and transfer quantum information, create entanglement within and with a specimen, and reveal previously inaccessible details on nanoscale quantum phenomena. This Roadmap outlines the current state of this rapidly evolving field, highlights key challenges and opportunities, and discusses future directions through a collection of topical sections prepared by leading experts.

cond-mat.mes-hall↗

arXiv2025

Benchmarking analytical electron ptychography methods for the low-dose imaging of beam-sensitive materials

This publication presents an investigation of the performance of different analytical electron ptychography methods for low-dose imaging. In particular, benchmarking is performed for two model-objects, monolayer MoS$_2$ and apoferritin, by means of multislice simulations. Specific attention is given to cases where the individual diffraction patterns remain sparse. After a first rigorous introduction to the theoretical foundations of the methods, an implementation based on the scan-frequency partitioning of calculation steps is described, permitting a significant reduction of memory needs and high sampling flexibility. By analyzing the role of contrast transfer and illumination conditions, this work provides insights into the trade-off between resolution, signal-to-noise ratio and probe focus, as is necessary for the optimization of practical experiments. Furthermore, important differences between the different methods are demonstrated. Overall, the results obtained for the two model-objects demonstrate that analytical ptychography is an attractive option for the low-dose imaging of beam-sensitive materials.

physics.app-ph↗