UltramicroscopyPub Date : 2025-03-06DOI: 10.1016/j.ultramic.2025.114122
L. Niermann, T. Niermann, M. Lehmann
{"title":"Dynamical diffraction effects of inhomogeneous strain fields investigated by scanning convergent electron beam diffraction and dark field electron holography","authors":"L. Niermann, T. Niermann, M. Lehmann","doi":"10.1016/j.ultramic.2025.114122","DOIUrl":"10.1016/j.ultramic.2025.114122","url":null,"abstract":"<div><div>Many material properties can be tuned by strain fields within the specimen. Examples range from mechanical properties of alloy hardening to electro-optical properties like emission wavelengths in semiconductor heterostructure quantum wells. While several transmission electron microscopy techniques for the measurements of these strain fields exists, these techniques typically neglect strain variations along the electron beam or try to mitigate their effects. Here we investigated the effects of these strain inhomogeneities along the beam direction under dynamical diffraction conditions. We performed scanning convergent beam electron diffraction and tilt series of dark-field electron holography measurements on an inclined layer structure, which exhibits a known 3D strain field. These measurements are compared with numerical multi-beam calculations, which allows to identify the depth of the strain inhomogeneity from the measured data. However, we observed a ambiguity of diffracted intensities stemming from a strain inhomogeneity which is symmetric with respect to the specimens mid-plane. The phases of the diffracted beams do not exhibit this symmetry. Furthermore, we also investigate the influence of experimental parameters like defocus and specimen curvature as well as relaxation effects on the measurements. We anticipate that the reported systematical investigations will form a starting point for the use of dynamical diffraction effects for more thorough measurements of 3D strain fields.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114122"},"PeriodicalIF":2.1,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580330","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-03-04DOI: 10.1016/j.ultramic.2025.114121
Adrien Moncomble , Damien Alloyeau , Maxime Moreaud , Abdelali Khelfa , Guillaume Wang , Nathaly Ortiz-Peña , Hakim Amara , Riccardo Gatti , Romain Moreau , Christian Ricolleau , Jaysen Nelayah
{"title":"aquaDenoising: AI-enhancement of in situ liquid phase STEM video for automated quantification of nanoparticles growth","authors":"Adrien Moncomble , Damien Alloyeau , Maxime Moreaud , Abdelali Khelfa , Guillaume Wang , Nathaly Ortiz-Peña , Hakim Amara , Riccardo Gatti , Romain Moreau , Christian Ricolleau , Jaysen Nelayah","doi":"10.1016/j.ultramic.2025.114121","DOIUrl":"10.1016/j.ultramic.2025.114121","url":null,"abstract":"<div><div>Automatic processing and full analysis of <em>in situ</em> liquid phase scanning transmission electron microscopy (LP-STEM) acquisitions are yet to be achievable with available techniques. This is particularly true for the extraction of information related to the nucleation and growth of nanoparticles (NPs) in liquid as several parasitic processes degrade the signal of interest. These degradations hinder the use of classical or state-of-the-art techniques making the understanding of NPs formation difficult to access. In this context, we propose aquaDenoising, a novel simulation-based deep neural framework to address the challenges of denoising LP-STEM images and videos. Trained on synthetic pairs of clean and noisy images obtained from kinematic-model-based simulations, we show that our model is able to achieve a fifteen-fold improvement in the signal-to-noise ratio of videos of gold NPs growing in water. The enhanced data unleash unprecedented possibilities for automatic segmentation and extraction of structures at different scales, from assemblies of objects down to the individual NPs with the same precision as manual segmentation performed by experts, but with higher throughput. The present denoising method can be easily adapted to other nanomaterials imaged in liquid media. All the codes developed in the present work are open and freely available.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114121"},"PeriodicalIF":2.1,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580329","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-03-04DOI: 10.1016/j.ultramic.2025.114119
Thibaud Denneulin, Benjamin Zingsem, Joseph Vas, Wen Shi, Luyan Yang, Michael Feuerbacher, Rafal E. Dunin-Borkowski
{"title":"Acquisition of object and temperature series in medium resolution off-axis electron holography with live drift correction","authors":"Thibaud Denneulin, Benjamin Zingsem, Joseph Vas, Wen Shi, Luyan Yang, Michael Feuerbacher, Rafal E. Dunin-Borkowski","doi":"10.1016/j.ultramic.2025.114119","DOIUrl":"10.1016/j.ultramic.2025.114119","url":null,"abstract":"<div><div>Collecting and averaging large datasets is a common practice in transmission electron microscopy to improve the signal-to-noise ratio. Averaging data in off-axis electron holography requires automated tools capable of correcting both the drift of the interference fringes and the drift of the specimen. This can be achieved either off-line, by post-processing hologram series, or on-line, through real-time microscope control. For on-line correction, a previously suggested method involves independently adjusting the position of the intereference fringes and the sample by controlling the beam tilt coils and the stage during hologram acquisition. In this study, we have implemented this on-line correction method in a Thermo Fisher Scientific Titan transmission electron microscope. The microscope is equipped with a piezo-enhanced CompuStage for positioning the sample with high precision. However, the control of the piezo stage via direct scripting is not supported. We first describe a workaround to enable automated sample position correction. We then demonstrate the benefits of live, program-controlled acquisitions for serial experiments in medium resolution off-axis electron holography. Application examples include the automatic acquisition of an object series such as a transistor array and an <em>in-situ</em> temperature series of magnetic skyrmions.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114119"},"PeriodicalIF":2.1,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143593126","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-27DOI: 10.1016/j.ultramic.2025.114124
Hannah R. Johnson, Legend Foster, Anikin Rae Domingo, Gregory P. Holland
{"title":"Negative stain TEM imaging of native spider silk protein superstructures","authors":"Hannah R. Johnson, Legend Foster, Anikin Rae Domingo, Gregory P. Holland","doi":"10.1016/j.ultramic.2025.114124","DOIUrl":"10.1016/j.ultramic.2025.114124","url":null,"abstract":"<div><div>Native <em>Latrodectus hesperus</em> (black widow) major ampullate spider silk proteins were imaged using negative stain transmission electron microscopy (NS-TEM) by isolating the silk protein hydrogel directly from the organism and solubilizing in urea. Heterogeneous micelle-like structures averaging 300 nm, similar to those imaged previously with CryoEM, were observed when stained with ammonium molybdate. A second smaller population averaging 50 nm was observed as well as large fibrils, highlighting the heterogeneous nature of the silk gland. The population of smaller silk protein micelles was enhanced at higher urea concentrations (5–8 M). This was further supported by dynamic light scattering (DLS), where two populations were observed at low urea concentrations while one small population dominated at high urea concentrations. The approach presented here provides a cost-effective route to imaging silk protein superstructures with conventional NS-TEM methods and may be applicable to other soft nanoparticle systems.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114124"},"PeriodicalIF":2.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143580328","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-26DOI: 10.1016/j.ultramic.2025.114123
Kristiaan H. Helfferich , Johannes D. Meeldijk , Marijn A. van Huis , Jessi E.S. van der Hoeven , Petra E. de Jongh
{"title":"Quantifying elemental colocation in nanostructured materials using energy-dispersive X-ray spectroscopy","authors":"Kristiaan H. Helfferich , Johannes D. Meeldijk , Marijn A. van Huis , Jessi E.S. van der Hoeven , Petra E. de Jongh","doi":"10.1016/j.ultramic.2025.114123","DOIUrl":"10.1016/j.ultramic.2025.114123","url":null,"abstract":"<div><div>Multicomponent nanostructured materials are key amongst others for energy and catalysis applications. The nanoscale proximity of different metals critically determines the performance of these functional materials. However, it is difficult to study the spatial distribution of different elements at the nanoscale, especially achieving a statistically relevant assessment. Additionally, common support materials like metal oxides are sensitive to electron beam damage when using high resolution local techniques, such as transmission electron microscopy. We present a robust strategy to quantitatively assess elemental distributions in 3D nanostructured beam-sensitive samples. Key elements are resin embedding, and elemental co-localisation building on a combination of electron tomography and energy-dispersive X-ray spectroscopy. We showcase the methodology with ∼ 3 nm Pd-Ni nanoparticles supported on mesoporous silica. Epoxy resin-embedding ensured sufficient sample stability under the electron beam for tomography-based quantification of different mano- and mesoscale elemental distributions in these samples. Reliable co-location results were obtained and practical guidelines are provided for acquisition and post-processing, relevant for elemental overlap analysis in multi-metallic samples.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114123"},"PeriodicalIF":2.1,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-24DOI: 10.1016/j.ultramic.2025.114120
William J. Davids, Mengwei He, Huma Bilal, Andrew J. Breen, Simon P. Ringer
{"title":"Using non-parametric statistical testing to quantify solute clustering in atom probe reconstructions","authors":"William J. Davids, Mengwei He, Huma Bilal, Andrew J. Breen, Simon P. Ringer","doi":"10.1016/j.ultramic.2025.114120","DOIUrl":"10.1016/j.ultramic.2025.114120","url":null,"abstract":"<div><div>Atom probe tomography (APT) is routinely used to investigate nano-scale solute architecture within multicomponent systems. However, there is no consensus on how to best quantify solute clustering within APT data. This contribution leverages recent developments in the field of non-parametric hypothesis testing of nearest-neighbour distributions to address this critical gap. We adapt a goodness-of-fit-type test statistic known as ‘the level of heterogeneity’ to quantitatively discern whether solute distributions exhibit clustering behaviour beyond what would be expected from a random distribution. Further, comparing APT datasets remains difficult due to the inability to directly compare their nearest-neighbour distributions. We present a method that leverages Monte-Carlo simulations, already used to calculate the non-parametric statistic, as a means of comparing APT data. The method is more powerful than comparing datasets through the Pearson coefficient, as is conventionally done.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114120"},"PeriodicalIF":2.1,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143548520","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-16DOI: 10.1016/j.ultramic.2025.114118
Robert M. Glaeser
{"title":"Commonsense and common nonsense opinions: PROSPECTS for further reducing beam damage in electron microscopy of radiation-sensitive specimens","authors":"Robert M. Glaeser","doi":"10.1016/j.ultramic.2025.114118","DOIUrl":"10.1016/j.ultramic.2025.114118","url":null,"abstract":"<div><div>Biological molecules are easily damaged by high-energy electrons, thus limiting the exposures that can be used to image such specimens by electron microscopy. It is argued here that many-electron, volume-plasmon excitations, which promptly transition into multiple types of single-electron ionization and excitation events, seem to be the predominant cause of damage in such materials. Although reducing the rate at which primary radiolysis occurs would allow one to record images that were much less noisy, many novel proposals for achieving this are unlikely to be realized in the near future, while others are manifestly ill-founded. As a result, the most realistic option currently is to more effectively use the available “budget” of electron exposure, i.e. to further improve the “dose efficiency” by which images are recorded. While progress in that direction is currently under way for both “conventional” (i.e. fixed-beam) and scanning EM, the former is expected to set a high standard for the latter to surpass.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114118"},"PeriodicalIF":2.1,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-16DOI: 10.1016/j.ultramic.2025.114116
Arda Genc , Justin Marlowe , Anika Jalil , Daniel Belzberg , Libor Kovarik , Phillip Christopher
{"title":"A versatile machine learning workflow for high-throughput analysis of supported metal catalyst particles","authors":"Arda Genc , Justin Marlowe , Anika Jalil , Daniel Belzberg , Libor Kovarik , Phillip Christopher","doi":"10.1016/j.ultramic.2025.114116","DOIUrl":"10.1016/j.ultramic.2025.114116","url":null,"abstract":"<div><div>Accurate and efficient characterization of nanoparticles (NPs), particularly regarding particle size distribution, is essential for advancing our understanding of their structure-property relationship and facilitating their design for various applications. In this study, we introduce a novel two-stage artificial intelligence (AI)-driven workflow for NP analysis that leverages prompt engineering techniques from state-of-the-art single-stage object detection and large-scale vision transformer (ViT) architectures. This methodology is applied to transmission electron microscopy (TEM) and scanning TEM (STEM) images of heterogeneous catalysts, enabling high-resolution, high-throughput analysis of particle size distributions for supported metal catalyst NPs. The model's performance in detecting and segmenting NPs is validated across diverse heterogeneous catalyst systems, including various metals (Ru, Cu, PtCo, and Pt), supports (silica (SiO<sub>2</sub>), γ-alumina (γ-Al<sub>2</sub>O<sub>3</sub>), and carbon black), and particle diameter size distributions with mean and standard deviations ranging from 1.6 ± 0.2 nm to 9.7 ± 4.6 nm. The proposed machine learning (ML) methodology achieved an average F1 overlap score of 0.91 ± 0.01 and demonstrated the ability to disentangle overlapping NPs anchored on catalytic support materials. The segmentation accuracy is further validated using the Hausdorff distance and robust Hausdorff distance metrics, with the 90th percent of the robust Hausdorff distance showing errors within 0.4 ± 0.1 nm to 1.4 ± 0.6 nm. Our AI-assisted NP analysis workflow demonstrates robust generalization across diverse datasets and can be readily applied to similar NP segmentation tasks without requiring costly model retraining.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114116"},"PeriodicalIF":2.1,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509280","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-16DOI: 10.1016/j.ultramic.2025.114117
Peter S. Neu , Eugene E. Krasovskii , Rudolf M. Tromp , Sense Jan van der Molen
{"title":"Bi-directional LEEM and eV-TEM spectroscopy on a graphene-hBN heterostack","authors":"Peter S. Neu , Eugene E. Krasovskii , Rudolf M. Tromp , Sense Jan van der Molen","doi":"10.1016/j.ultramic.2025.114117","DOIUrl":"10.1016/j.ultramic.2025.114117","url":null,"abstract":"<div><div>Van der Waals heterostacks can exhibit emergent properties as a result of the coupling between the individual layers stacked. Here we focus on heterostacks of graphene and hBN, and study both coherent electron resonances (or unoccupied states) and inelastic losses. For this, we measure electron reflection and transmission spectra of the stack, as a function of electron energy. Special attention is paid to the symmetry upon flipping the heterostack, i.e., whether the electrons are first incident on the graphene or on the hBN surface: whereas electron reflection may be sensitive to sample orientation, electron transmission should not. Experimentally, we compare LEEM (reflection) and eV-TEM (transmission) IV spectra measured on free-standing graphene-hBN heterostacks with either the graphene or hBN side facing the LEEM objective lens. Resonances and inelastic loss are first modeled with the help of a simple wave interference toy model inspired by optics. More advanced calculations are performed to obtain the spatially resolved density of unoccupied states in the heterostack. We relate these calculations to the measured spectra, taking into account the finite probing depth of the reflected electron beam.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114117"},"PeriodicalIF":2.1,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
UltramicroscopyPub Date : 2025-02-09DOI: 10.1016/j.ultramic.2025.114115
Bavley Guerguis , Ramya Cuduvally , Richard J.H. Morris , Gabriel Arcuri , Brian Langelier , Nabil Bassim
{"title":"Erratum to \"The impact of electric field strength on the accuracy of boron dopant quantification in silicon using atom probe tomography\"","authors":"Bavley Guerguis , Ramya Cuduvally , Richard J.H. Morris , Gabriel Arcuri , Brian Langelier , Nabil Bassim","doi":"10.1016/j.ultramic.2025.114115","DOIUrl":"10.1016/j.ultramic.2025.114115","url":null,"abstract":"","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"271 ","pages":"Article 114115"},"PeriodicalIF":2.1,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143400325","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}