UltramicroscopyPub Date : 2025-04-26DOI: 10.1016/j.ultramic.2025.114153
BG Mendis
{"title":"On the impulse approximation in electron Compton scattering","authors":"BG Mendis","doi":"10.1016/j.ultramic.2025.114153","DOIUrl":"10.1016/j.ultramic.2025.114153","url":null,"abstract":"<div><div>Electronic structure measurement via Compton scattering requires the impulse approximation to be satisfied. This states that the inelastic collision time is short, so that the ‘secondary’ electron ejected out of the atom is effectively free of the crystal potential. The robustness of the impulse approximation is tested for boron nitride and aluminium using momentum-resolved electron energy loss spectroscopy. Reliable (with respect to impulse approximation) electronic structure information is obtained for Compton peak energies at ∼250 eV energy loss or higher. These experimental results are validated using a simple Kronig-Penney model of the secondary electron travelling through the crystal. For loosely bound valence electrons the impulse approximation is satisfied when the Compton peak energy is significantly larger than the mean inner potential of the crystal. This criterion provides a straightforward estimate of the experimental conditions required for extracting reliable Compton data from any given material.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114153"},"PeriodicalIF":2.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895965","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 : 2025-04-18DOI: 10.1016/j.ultramic.2025.114150
Sarah Schroeder , Koen Dewettinck , Volker Heinz , Ute Bindrich , Dana Middendorf , Knut Franke
{"title":"Opportunities and challenges to determine surface free energy of chocolates on microscopic scale from atomic force microscopy adhesion measurements","authors":"Sarah Schroeder , Koen Dewettinck , Volker Heinz , Ute Bindrich , Dana Middendorf , Knut Franke","doi":"10.1016/j.ultramic.2025.114150","DOIUrl":"10.1016/j.ultramic.2025.114150","url":null,"abstract":"<div><div>Surface free energy (SFE) is an important surface property in food processing as it determines the wettability of solid surfaces or the interaction of mould surfaces and chocolate during the moulding process. High-resolution information about SFE could be useful to understand gloss inhomogeneities of chocolates after de-moulding. SFE is connected with adhesion properties. Thus, Atomic force microscopy (AFM) adhesion measurements can be applied to determine SFE of a solid surface at microscopic scale. For this purpose, AFM tips were functionalized to modify their SFE and used for adhesion measurements at three different chocolate gloss areas (matt, glossy and homogenous) via AFM force maps. Influence of relevant parameters such as surface roughness, contact area, relative humidity, and SFE of functionalized tips was considered. Two different mathematical approaches based on Johnson-Kendall-Roberts theory were used to calculate SFE from adhesion values. The measured adhesion values showed variations depending on functionalized tip and chocolate gloss area. The results showed a difference in adhesion and, consequently, SFE in the different gloss areas with gloss > homogenous > matt. However, SFE obtained from adhesion forces were not decisive enough to enable a direct correlation with SFE data from contact angle measurements at the same area.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114150"},"PeriodicalIF":2.1,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143855695","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 : 2025-04-18DOI: 10.1016/j.ultramic.2025.114148
Ilya A. Morozov, Roman I. Izyumov
{"title":"Influence of experimental conditions on apparent AFM tip-surface contact in air","authors":"Ilya A. Morozov, Roman I. Izyumov","doi":"10.1016/j.ultramic.2025.114148","DOIUrl":"10.1016/j.ultramic.2025.114148","url":null,"abstract":"<div><div>Accurate determination of the onset of the contact between the atomic force microscope (AFM) tip and the surface in force measurements is necessary both for calculating the constants of non-contact interactions and for determining the structural and mechanical properties of the materials. In an air environment the contact is preceded by a rapid jump of the tip to the surface due to attractive forces. If a surface is not deformed by a probe of a given stiffness, the end of the jump (minimum of the deflection of the cantilever) is taken as the onset of the contact. In this work, it is shown that the tip contacts with the deformable surface before the completion of the jump. It is reasonable to use the point of the extreme deflection velocity as the onset of the contact. A dynamic mass-spring model of the interaction of the tip with the viscoelastic material has shown that the high deflection velocity and the low rate of data acquisition (bandwidth) are the reasons for significant errors in determining the contact from the experimental force curve. In the most cases, the observed contact point is lower than the actual one (under certain conditions, the opposite situation is also possible) and the measurement error is at least 50 % (depending on the experimental settings, the properties of the probe and the material).</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114148"},"PeriodicalIF":2.1,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870563","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":"Capacitance compensation on a double-barrel nanopipette for improving current detection of scanning ion conductance microscopy","authors":"Futoshi Iwata , Naoto Fukuzawa , Hitoshi Inomata , Kenta Nakazawa , Toshi Nagata , Hideya Kawasaki , Osamu Hoshi","doi":"10.1016/j.ultramic.2025.114149","DOIUrl":"10.1016/j.ultramic.2025.114149","url":null,"abstract":"<div><div>We developed a method to improve the current-detection response of scanning ion conduction microscopy (SICM) using a double-barrel nanopipette. By detecting the difference between the two signals from each channel, capacitive currents can be canceled out, resulting in an improved ion current detection response and reduced imaging time in bias-modulated scanning ion conductance microscopy operated with AC bias voltages (BM-SICM). Furthermore, this method can reduce the synchronized capacitive current noise of two adjacent channels of a double-barrel nanopipette by canceling each other via a differential operation. Therefore, an improved detection signal was achieved even in the SICM operated with a DC bias voltage by reducing the noise from the piezoelectric scanner. As demonstrated by the proposed method, chromosomes that were difficult to observe owing to their strong negative charges were clearly imaged in the BM-SICM operated with an AC bias voltage without artifacts caused by surface charging. Additionally, in SICM operating with a DC bias voltage, dynamic interaction among an intracellular short rod, <em>Listeria monocytogenes</em>, and Caco-2 human enterocyte-like cells was successfully observed.</div></div>","PeriodicalId":23439,"journal":{"name":"Ultramicroscopy","volume":"273 ","pages":"Article 114149"},"PeriodicalIF":2.1,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864533","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 : 2025-04-08DOI: 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}
{"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 : 2025-03-15DOI: 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}