UltramicroscopyPub Date : 2025-04-08DOI: 10.1016/j.ultramic.2025.114136
Pengfei Lin, Kuan Lu, ChaBum Lee
{"title":"A novel method for through-silicon via characterization based on diffraction fringe analysis","authors":"Pengfei Lin, Kuan Lu, ChaBum Lee","doi":"10.1016/j.ultramic.2025.114136","DOIUrl":"10.1016/j.ultramic.2025.114136","url":null,"abstract":"<div><div>The precision metrology of through-hole silicon via (TSV) in the semiconductor industry has remained a critical challenge as its critical dimension (CD) reduces. In this letter, we report a novel method for TSV geometric feature measurement and characterization. By illuminating a collimated infrared laser beam to the TSV and then analyzing the TSV edge-induced diffraction interferometric fringe patterns, multiple geometric information of the TSV could be characterized, establishing its database. This computational approach to TSV characterization was validated by experiments. Being non-destructive and easy to deploy, this method provides a low cost and high efficiency solution for TSV metrology.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"272 ","pages":"Article 114136"},"PeriodicalIF":2.1,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143792586","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 : 2025-04-05DOI: 10.1016/j.ultramic.2025.114137
Desheng Ma , Steven E. Zeltmann , Chenyu Zhang , Zhaslan Baraissov , Yu-Tsun Shao , Cameron Duncan , Jared Maxson , Auralee Edelen , David A. Muller
{"title":"Emittance minimization for aberration correction I: Aberration correction of an electron microscope without knowing the aberration coefficients","authors":"Desheng Ma , Steven E. Zeltmann , Chenyu Zhang , Zhaslan Baraissov , Yu-Tsun Shao , Cameron Duncan , Jared Maxson , Auralee Edelen , David A. Muller","doi":"10.1016/j.ultramic.2025.114137","DOIUrl":"10.1016/j.ultramic.2025.114137","url":null,"abstract":"<div><div>Precise alignment of the electron beam is critical for successful application of scanning transmission electron microscopes (STEM) to understanding materials at atomic level. Despite the success of aberration correctors, aberration correction is still a complex process. Here we approach aberration correction from the perspective of accelerator physics and show it is equivalent to minimizing the emittance growth of the beam, the span of the phase space distribution of the probe. We train a deep learning model to predict emittance growth from experimentally accessible Ronchigrams. Both simulation and experimental results show the model can capture the emittance variation with aberration coefficients accurately. We further demonstrate the model can act as a fast-executing function for the global optimization of the lens parameters. Our approach enables new ways to quickly quantify and automate aberration correction that takes advantage of the rapid measurements possible with high-speed electron cameras. In part II of the paper, we demonstrate how the emittance metric enables rapid online tuning of the aberration corrector using Bayesian optimization.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114137"},"PeriodicalIF":2.1,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143821413","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 : 2025-04-04DOI: 10.1016/j.ultramic.2025.114138
Desheng Ma , Steven E. Zeltmann , Chenyu Zhang , Zhaslan Baraissov , Yu-Tsun Shao , Cameron Duncan , Jared Maxson , Auralee Edelen , David A. Muller
{"title":"Emittance Minimization for Aberration Correction II: Physics-informed Bayesian Optimization of an Electron Microscope","authors":"Desheng Ma , Steven E. Zeltmann , Chenyu Zhang , Zhaslan Baraissov , Yu-Tsun Shao , Cameron Duncan , Jared Maxson , Auralee Edelen , David A. Muller","doi":"10.1016/j.ultramic.2025.114138","DOIUrl":"10.1016/j.ultramic.2025.114138","url":null,"abstract":"<div><div>Aberration-corrected Scanning Transmission Electron Microscopy (STEM) has become an essential tool in understanding materials at the atomic scale. However, tuning the aberration corrector to produce a sub-Ångström probe is a complex and time-costly procedure, largely due to the difficulty of precisely measuring the optical state of the system. When measurements are both costly and noisy, Bayesian methods provide rapid and efficient optimization. To this end, we develop a Bayesian approach to fully automate the process by minimizing a new quality metric, beam emittance, which is shown to be equivalent to performing aberration correction. In part I, we derived several important properties of the beam emittance metric and trained a deep neural network to predict beam emittance growth from a single Ronchigram. Here we use this as the black box function for Bayesian Optimization and demonstrate automated tuning of simulated and real electron microscopes. We explore different surrogate functions for the Bayesian optimizer and implement a deep neural network kernel to effectively learn the interactions between different control channels without the need to explicitly measure a full set of aberration coefficients. Both simulation and experimental results show the proposed method outperforms conventional approaches by achieving a better optical state with a higher convergence rate.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114138"},"PeriodicalIF":2.1,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143821412","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 : 2025-04-01DOI: 10.1016/j.ultramic.2025.114135
Alan J. Craven , Bianca Sala , Donald A. MacLaren , Sam McFadzean , Bernhard Schaffer , Ian MacLaren
{"title":"Splicing dual-range EELS spectra: Identifying and correcting artefacts","authors":"Alan J. Craven , Bianca Sala , Donald A. MacLaren , Sam McFadzean , Bernhard Schaffer , Ian MacLaren","doi":"10.1016/j.ultramic.2025.114135","DOIUrl":"10.1016/j.ultramic.2025.114135","url":null,"abstract":"<div><div>In dual or multiple range electron energy loss spectroscopy, splicing the low loss spectra together with core loss ranges allows Fourier-log deconvolution of the entire energy range. However, because of the huge intrinsic dynamic range in EELS, the intensity at the splice point in a low loss spectrum is typically small, meaning that even weak or subtle artefacts can have big effects. Three main sources of artefacts in a Gatan GIF Quantum system have been investigated: non-uniformity of energy dispersion caused by aberrations in the spectrometer optics, stray scattering in the detector chamber, and small differences between the responsivity of the different detector quadrants. We present methods to measure, quantify and correct these artefacts. Ideally, the ratio for scaling at the splice should be the ratio of integration times. Prior to correction, the scaling factor is found to be about 15 % less than the exposure or time ratio and is dependent on the specimen thickness. After correction, the discrepancies are less than 0.5 %. This allows quantitative comparison of data taken at different points in time, even after major system changes, provided suitable artefact-correction datasets are taken. Whilst the detail is specific to one particular instrument, the principles are also applicable to newer spectrometers, including those with direct electron detectors.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"272 ","pages":"Article 114135"},"PeriodicalIF":2.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143785528","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 : 2025-03-15DOI: 10.1016/j.ultramic.2025.114133
Yong Ding , Yuzi Liu , Yu Chen , Meilin Liu , Zhong Lin Wang
{"title":"Direct observation of oxygen vacancy ordering evolution in cerium oxide at varying concentrations via high-resolution transmission electron microscopy","authors":"Yong Ding , Yuzi Liu , Yu Chen , Meilin Liu , Zhong Lin Wang","doi":"10.1016/j.ultramic.2025.114133","DOIUrl":"10.1016/j.ultramic.2025.114133","url":null,"abstract":"<div><div>Under illumination by a 300 keV electron beam, oxygen vacancy ordering structures are induced within cerium oxide grains. Our high-resolution transmission electron microscopy (HRTEM) study, supported by image simulation, reveals the evolution of these structures as vacancy concentration increases. The observed fluorite-type superlattice structures are identified as CeO<sub>1.825</sub>, CeO<sub>1.75</sub>, Ce<sub>2</sub>O<sub>3</sub>, displaying a gradient in oxygen vacancy concentration moving away from the grain surface. Correspondingly, the structural sequence transitions from Ce<sub>2</sub>O<sub>3</sub> to CeO<sub>1.75</sub> and then to CeO<sub>1.825</sub>. Without the constraints of surrounding grains, fluorite-type Ce<sub>2</sub>O<sub>3</sub> nanocrystals show a preference for transformation into an A-type trigonal structure. Notably, at temperatures up to 200°C, only the perfect fluorite structure is observed. Structural models were validated through both [110] and [001] projections. Our findings further confirm lattice expansion associated with local oxygen vacancy enrichment, which can be compensated by the formation of stacking faults, where a {111} oxygen plane is lost at defect sites.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"272 ","pages":"Article 114133"},"PeriodicalIF":2.1,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654834","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}
{"title":"Quantitative evaluation of local magnetic property using magnetic domain wall width measurement with tilt-scan averaged DPC STEM","authors":"Yoshiki O. Murakami , Takehito Seki , Koudai Tabata , Yuichi Ikuhara , Naoya Shibata","doi":"10.1016/j.ultramic.2025.114132","DOIUrl":"10.1016/j.ultramic.2025.114132","url":null,"abstract":"<div><div>Identifying the one-to-one relationship between microstructures and magnetic properties is crucial for improving the coercivity of permanent magnets. Magnetic domain wall (DW) is an important local magnetic structure, whose width is closely related to the local magnetic properties of the magnets. Unfortunately, due to the limitations of conventional experimental methods, direct and precise measurements of nanoscale DW widths have been challenging. However, recent advancements in differential phase contrast scanning transmission electron microscopy (DPC STEM) have enabled direct imaging of magnetic field distribution down to atomic dimensions. In this study, the precise measurement of the DW width in Nd-Fe-B type magnets using high-resolution DPC images in a magnetic field-free environment was demonstrated. The change in DW width with respect to the change in the magnet's local composition was measured. Moreover, we can estimate local magnetic properties such as exchange stiffness and magnetocrystalline anisotropy from the DW width. Therefore, DPC STEM can be used to evaluate the local magnetic properties of magnets with complex microstructures.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"272 ","pages":"Article 114132"},"PeriodicalIF":2.1,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143697021","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 : 2025-03-06DOI: 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}