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Substrate matters: Coupled phonon modes of a spherical particle on a substrate probed with EELS 衬底问题:用EELS探测衬底上球形粒子的耦合声子模式
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-09-01 DOI: 10.1016/j.ultramic.2025.114229
Ka Yin Lee , Elliot K. Beutler , Tifany Q. Crisolo , David J. Masiello , Maureen J. Lagos
Using vibrational electron energy loss spectroscopy (vib-EELS) combined with numerical modeling, we investigate the physical mechanisms governing the phonon coupling between a spherical particle sustaining multipolar surface phonon modes and an underlying thin film. Depending upon their dielectric composition, a variety of hybrid phonon modes arise in the EEL spectrum due to the interaction between polarization charges in the particle and film. Mirror charge effects and phonon mode hybridization are the active mechanisms acting on dielectric and metallic-type films, respectively. Processes beyond dipole-dipole interactions are required to describe the sphere-film coupling.
利用振动电子能量损失谱(vib-EELS)与数值模拟相结合,研究了维持多极表面声子模式的球形粒子与底层薄膜之间声子耦合的物理机制。根据它们的介电成分,由于粒子和薄膜中的极化电荷之间的相互作用,在EEL光谱中出现了各种混合声子模式。镜像电荷效应和声子模式杂化分别是作用于介质型和金属型薄膜的活性机制。描述球膜耦合需要超越偶极-偶极相互作用的过程。
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引用次数: 0
A new EBSD indexing method with enhanced grain boundary indexing performance using a three-dimensional parameter space 基于三维参数空间的EBSD标引方法提高了晶界标引性能
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-26 DOI: 10.1016/j.ultramic.2025.114227
Fan Peng , Xuemei Song , Yiling Huang , Xingyu Jin , Yuqing Jiang , Yue Sun , Yi Zeng
Electron backscatter diffraction (EBSD) is an important technique based on the scanning electron microscope (SEM) that provides a wide range of crystallographic information. There are limited available pattern indexing methods and most of them are mastered by commercial instrument manufacturers, which may probably restrict the sharing and development of indexing techniques. In this study, we present a new EBSD pattern indexing method based on a three-dimensional parameter space. This method extends the characterization of characteristic triangles into a three-dimensional parameter space. This work details the procedure of the new indexing algorithm. The utility of this new method is demonstrated using experimental patterns captured from a cubic yttria-stabilized zirconia (YSZ) bulk sample. Compared with commercial indexing results, the new method shows excellent consistency and achieves better indexing performance at grain boundaries.
电子背散射衍射(EBSD)是基于扫描电子显微镜(SEM)的一项重要技术,它提供了广泛的晶体学信息。现有的模式标引方法有限,且大多为商业仪器制造商所掌握,这可能会制约标引技术的共享和发展。本文提出了一种基于三维参数空间的EBSD模式索引方法。该方法将特征三角形的表征扩展到三维参数空间。本文详细介绍了新索引算法的实现过程。利用从立方氧化钇稳定氧化锆(YSZ)散装样品中捕获的实验图案证明了这种新方法的实用性。与商业标引结果相比,该方法一致性好,在晶界处标引性能更好。
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引用次数: 0
Differentiating electron diffuse scattering via 4D-STEM spatial fluctuation and correlation analysis in complex FCC alloys 基于4D-STEM空间波动和相关分析的复杂FCC合金中电子漫射的鉴别
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-25 DOI: 10.1016/j.ultramic.2025.114228
Po-Cheng Kung , Rui Feng , Peter Liaw , Jian-Min Zuo , Jessica Krogstad
Complex face-centered-cubic (FCC) alloys frequently display chemical short-range ordering (CSRO), which can be detected through the analysis of diffuse scattering. However, the interpretation of diffuse scattering is complicated by the presence of defects and thermal diffuse scattering, making it extremely challenging to distinguish CSRO using conventional scattering techniques. This complexity has sparked intense debates regarding the origin of specific diffuse-scattering signals, such as those observed at 1/3{422} and 1/2{311} positions. To address this challenge, we introduce the method of spatial fluctuation and correlation (FluCor) analysis of local diffuse scattering captured using Four-Dimensional Scanning Transmission Electron Microscopy (4D-STEM). We demonstrate our methodology using a solution-treated (CrCoNi)93Al4Ti2Nb medium-entropy alloy (MEA) and show that the FluCor analysis can differentiate diffuse scattering of different origins. The results reveal two sets of overlapping diffuse-scattering signals at the 1/3{422} and 1/2{311} positions in the studied MEA and link both to non-CSRO origins. Specifically, the heterogeneous-domain diffuse-scattering signals are attributed to nanoscale planar defects, while the homogeneous diffuse-scattering of the matrix is best explained by thermal-diffuse scattering. The principles underlying our fluctuation and correlation analysis of diffuse scattering are general and broadly applicable to order-disordered crystals, including various complex alloy systems. This versatility promises to yield valuable insights into the interplay between microstructural characteristics and CSRO behavior in a wide range of materials, potentially resolving long-standing debates in the field.
复杂面心立方(FCC)合金经常显示化学短程有序(CSRO),这可以通过漫射散射分析来检测。然而,漫射散射的解释由于缺陷和热漫射的存在而变得复杂,使得使用传统的散射技术来区分CSRO极具挑战性。这种复杂性引发了关于特定扩散散射信号起源的激烈争论,例如在1/3{422}和1/2{311}位置观测到的信号。为了解决这一挑战,我们引入了四维扫描透射电子显微镜(4D-STEM)捕获的局部漫射散射的空间波动和相关(FluCor)分析方法。我们用溶液处理的(CrCoNi)93Al4Ti2Nb中熵合金(MEA)证明了我们的方法,并表明fluor分析可以区分不同来源的漫射散射。结果显示,在研究的MEA的1/3{422}和1/2{311}位置上存在两组重叠的扩散散射信号,并将它们与非csro起源联系起来。具体来说,异质域扩散散射信号归因于纳米级平面缺陷,而基体的均匀扩散散射最好用热扩散散射来解释。我们的漫射散射涨落和相关分析的基本原理是通用的,广泛适用于有序无序晶体,包括各种复杂合金体系。这种多功能性有望对各种材料的微观结构特征和CSRO行为之间的相互作用产生有价值的见解,可能解决该领域长期存在的争论。
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引用次数: 0
Improving the low-dose performance of aberration correction in single sideband ptychography 提高单边带成像像差校正的低剂量性能
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-23 DOI: 10.1016/j.ultramic.2025.114225
Songge Li , Nicolas Gauquelin , Hoelen L. Lalandec Robert , Arno Annys , Chuang Gao , Christoph Hofer , Timothy J. Pennycook , Jo Verbeeck
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 the invested electron dose, in part due to the necessity of phase unwrapping. In this work, we thus propose two strategies to improve the 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.
分析电子平面摄影的单边带(SSB)框架可以解释探针形成透镜引起的残余几何像差的存在。然而,这种像差校正方法的精度对所投入的电子剂量高度敏感,部分原因是相位展开的必要性。在这项工作中,我们因此提出了两种策略来提高在低剂量条件下的性能:在侧带内限制相位展开和只选择充分展开的侧带来计算像差系数。通过单层二硒化钨(WSe2)的模拟和实验4D-STEM数据集的SSB重建,验证了这些策略。对比结果表明,泊松噪声耐受性显著提高,使像差校正在低剂量成像中更加稳健和可靠。
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引用次数: 0
Impact of electron beam propagation on high-resolution quantitative chemical analysis of 1-nm-wide GaN/AlGaN quantum wells 电子束传播对1纳米宽GaN/AlGaN量子阱高分辨率定量化学分析的影响
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-19 DOI: 10.1016/j.ultramic.2025.114222
Florian Castioni , Patrick Quéméré , Sergi Cuesta , Vincent Delaye , Pascale Bayle-Guillemaud , Eva Monroy , Eric Robin , Nicolas Bernier
Recent advancements in high-resolution spectroscopy analyses within the scanning transmission electron microscope (STEM) have paved the way for measuring the concentration of chemical species in crystalline materials at the atomic scale. However, several artifacts complicate the direct interpretation of experimental data. For instance, in the case of energy-dispersive X-ray (EDX) spectroscopy, the linear dependency of local X-ray emission on composition is disrupted by channeling effects and cross-talk during electron beam propagation. To address these challenges, it becomes necessary to adopt an approach that combines experimental data with inelastic scattering simulations. This method aims to account for the effects of electron beam propagation on X-ray emission, essentially determining the quantity and the spatial origin of the collected signal. In this publication, we propose to assess the precision and sensitivity limits of this approach in a practical case study involving a focused ion beam (FIB)-prepared III-N multilayers device. The device features nominally pure ∼1.5-nm-wide GaN quantum wells surrounded by AlGaN barriers containing a low concentration of aluminum (∼5 at%). By employing atomic-scale EDX acquisitions based on the averaging of more than several thousand frames, calibrated ζ factors combined with a multilayer X-ray absorption correction model for quantification, and by comparing the X-ray radiation obtained from the quantum well with a reference 10-nm-wide structure, we demonstrate that the quantitative impact of beam propagation on chemical composition can be precisely accounted for, resulting in a composition sensitivity at the atomic scale as low as ±0.25 at%. Finally, practical aspects to achieve this high precision level are discussed, particularly in terms of inelastic multislice simulation, uncertainty determination, and sample quality.
扫描透射电子显微镜(STEM)中高分辨率光谱分析的最新进展为在原子尺度上测量晶体材料中化学物质的浓度铺平了道路。然而,一些人为因素使实验数据的直接解释复杂化。例如,在能量色散x射线(EDX)光谱学中,电子束传播过程中的通道效应和串扰破坏了局部x射线发射对成分的线性依赖。为了解决这些挑战,有必要采用一种将实验数据与非弹性散射模拟相结合的方法。该方法旨在解释电子束传播对x射线发射的影响,本质上是确定收集信号的数量和空间来源。在这篇文章中,我们建议在涉及聚焦离子束(FIB)制备的III-N多层器件的实际案例研究中评估该方法的精度和灵敏度限制。该器件具有名义上纯的~ 1.5 nm宽的GaN量子阱,被含有低浓度铝(~ 5 at%)的AlGaN势垒包围。通过采用原子尺度的EDX采集,基于超过几千帧的平均,校准ζ因子结合多层x射线吸收校正模型进行量化,并通过比较从量子阱获得的x射线辐射与参考10纳米宽结构,我们证明了光束传播对化学成分的定量影响可以精确地解释。导致在原子尺度上的成分灵敏度低至±0.25 at%。最后,讨论了实现这种高精度水平的实际方面,特别是在非弹性多片模拟,不确定性确定和样品质量方面。
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引用次数: 0
Breakdown and polarization contrasts in ferroelectric devices observed by operando laser-based photoemission electron microscopy with the AC/DC electrical characterization system 利用交流/直流电学表征系统,利用operando激光光电发射电子显微镜观察铁电器件的击穿和极化对比
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-11 DOI: 10.1016/j.ultramic.2025.114221
Hirokazu Fujiwara , Yuki Itoya , Masaharu Kobayashi , Cédric Bareille , Toshiyuki Taniuchi
We have developed an operando laser-based photoemission electron microscope (laser-PEEM) with a ferroelectric characterization system. A Sawyer-Tower circuit was implemented to measure the polarization–voltage (PV) characteristics of ferroelectric devices. Using this system, we successfully obtained the well-defined PV hysteresis loops for a ferroelectric capacitor incorporating Hf0.5Zr0.5O2 (HZO), reproducing the typical field-cycling characteristics of HZO capacitors. After dielectric breakdown caused by field-cycling stress, we visualized a conduction filament through the top electrode without any destructive processing. Additionally, we successfully observed polarization contrast through the top electrode of an oxide semiconductor (InZnOx). These results indicate that our operando laser-PEEM system is a powerful tool for visualizing conduction filaments after dielectric breakdown, the ferroelectric polarization contrasts, and electronic state distribution of materials implemented in ferroelectric devices, including ferroelectric field-effect transistors and ferroelectric tunnel junctions.
我们开发了一种具有铁电表征系统的基于operando激光的光电电子显微镜(laser-PEEM)。采用索耶-塔式电路测量铁电器件的极化电压特性。利用该系统,我们成功地获得了含有HZO (Hf0.5Zr0.5O2)的铁电电容器的P-V磁滞回线,再现了HZO电容器的典型场循环特性。在场循环应力引起的介质击穿后,我们在没有任何破坏性处理的情况下,通过顶部电极看到了导电丝。此外,我们成功地通过氧化物半导体(InZnOx)的顶电极观察到极化对比。这些结果表明,我们的operando激光- peem系统是一个强大的工具,用于可视化介电击穿后的导电丝,铁电极化对比和铁电器件中材料的电子态分布,包括铁电场效应晶体管和铁电隧道结。
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引用次数: 0
Fourier-based multiple-slice reconstruction in cryo-electron tomography 低温电子断层扫描中基于傅里叶的多层重建
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-08-10 DOI: 10.1016/j.ultramic.2025.114223
Ranhao Zhang , Yuan Shen , Xueming Li
A tomogram is reconstructed from the micrographs of the tilt series using cryo-electron tomography (cryoET). Reconstruction frequently integrates image processing steps, such as filtering and contrast transfer function (CTF) correction, to support the downstream analysis of cellular and viral structures. Most image processing steps are based on Fourier space analysis, which is theoretically more efficient to be implemented in Fourier space than in real space. However, the substantial dimensions of tomograms present significant challenges for reconstruction and processing in Fourier space. Consequently, real-space reconstruction is prevalent in current practice. In this study, we proposed a Fourier-space algorithm for tomogram reconstruction, named MUltiple Slice Technique (MUST). MUST considers a tomogram composed of multiple parallel slices, with each slice independently reconstructed in Fourier space. A weighting strategy was used to enable MUST to achieve reconstruction compatible with real-space methods, including weighted back-projection (WBP) and the simultaneous iterative reconstruction technique (SIRT). A three-dimensional CTF model was formulated as pairs of conjugate central paraboloids in Fourier space and subsequently implemented for CTF correction in MUST. Alias-free reconstruction and pixel-level parallel computation are key features of MUST, demonstrated through tomogram-based subtomogram averaging at near-atomic resolutions.
利用低温电子断层扫描(cryoET)从倾斜序列的显微照片重建层析图。重建通常集成图像处理步骤,如滤波和对比度传递函数(CTF)校正,以支持细胞和病毒结构的下游分析。大多数图像处理步骤都是基于傅里叶空间分析,理论上在傅里叶空间中实现比在实际空间中实现更有效。然而,层析图的大尺寸对傅里叶空间的重建和处理提出了重大挑战。因此,在当前的实践中,实空间重构是非常普遍的。在本研究中,我们提出了一种用于层析图重建的傅里叶空间算法,称为多重切片技术(MUltiple Slice Technique, MUST)。MUST考虑由多个平行切片组成的层析图,每个切片在傅里叶空间中独立重建。采用加权策略使MUST能够实现与实空间方法(包括加权反投影(WBP)和同步迭代重建技术(SIRT))兼容的重建。三维CTF模型在傅里叶空间中被表述为一对共轭中心抛物面,随后在MUST中实现CTF校正。无别名重建和像素级并行计算是MUST的关键特征,通过近原子分辨率的基于层析图的子层析图平均来证明。
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引用次数: 0
Resonant scattering in low energy electron diffraction: Bi/Ni(111) 低能电子衍射中的共振散射:Bi/Ni(111)
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-07-28 DOI: 10.1016/j.ultramic.2025.114220
Bene Poelsema, Martina Tsvetanova, Harold J.W. Zandvliet, Arie van Houselt
We report Low Energy Electron Diffraction (LEED) diffraction patterns measured at energies up to 50 eV for a monolayer thick Bi film on Ni(111). Surprisingly, the intensity versus energy profiles of several from the ten unique (i.e., symmetry-independent) sets of spots show finite but pertinent intensity, each only at a well-defined energy. These are attributed to resonant scattering, involving transient capture in eigenstates of the image potential, followed by (multiple) scattering into the vacuum. By its nature, transient capture occurs closely before the energy crosses the Ewald sphere for each considered channel. These energies are one-to-one connected with the corresponding lattice parameters of the Bi-film with its centered rectangular structure, commensurate along Ni[11–2] and high order commensurate along Ni[-110].
In addition, a couple of more intense regular spots show anomalously high intensity at the low energy side upon crossing the Ewald sphere. This feature is attributed to resonant scattering as well. We claim that so far grossly disregarded resonant scattering is a general phenomenon and should be considered in very low energy LEED-IV structural analysis.
The intensity versus energy profile of the (0 2) peak does not show obvious evidence for resonant scattering but instead reveals that the Bi film is built up by long (> 20 nm) and narrow (<< 20 nm), translationally shifted domains, oriented along the [-110] azimuth.
我们报道了Ni(111)上单层厚Bi薄膜在能量高达50 eV时的低能电子衍射(LEED)衍射图。令人惊讶的是,十个独特的(即,对称无关的)光斑集合中的几个的强度与能量分布显示有限但相关的强度,每个只在一个定义良好的能量。这些都归因于共振散射,涉及图像势的本征态的瞬态捕获,随后(多次)散射到真空中。就其性质而言,瞬态捕获发生在能量穿过每个通道的埃瓦尔德球之前。这些能量与具有中心矩形结构的双膜相应的晶格参数呈一一对应关系,沿Ni[11-2]成正比,沿Ni[-110]成高阶成正比。此外,一对更强烈的规则斑点在穿过埃瓦尔德球时,在低能侧表现出异常的高强度。这一特点也归因于共振散射。我们认为,到目前为止,被严重忽视的共振散射是一种普遍现象,应该在极低能量的LEED-IV结构分析中加以考虑。(02)峰的强度-能量分布图没有显示出明显的共振散射证据,而是表明Bi膜是由长(>;20 nm)和窄(<<;20 nm),平移位移域,沿[-110]方位角取向。
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引用次数: 0
Observation of domain morphology in twisted antimonene layers via moiré superlattice contrast with low energy electron microscopy 用低能电子显微镜观察扭曲锑烯层的畴形态
IF 2 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-07-27 DOI: 10.1016/j.ultramic.2025.114219
Mariusz Gołębiowski , Piotr Dróżdż , Ryszard Zdyb
Using low energy electron microscopy we investigate the origin of the contrast between domains in a heterostructure composed of twisted two-dimensional antimonene layers. The contrast is observed in the bright-field microscopy mode under normal incidence of the electron beam. The heterostructure consists of a single-domain β phase grown on a top of two-domain α phase antimonene on a W(110) surface. We show that the observed contrast is due to the formation of two different moiré superlattices and it directly reflects the two-domain structure of α antimonene. We also demonstrate that the contrast depends on the relative symmetry and crystallography of two moiré patterns.
利用低能电子显微镜,我们研究了由扭曲的二维反二烯层组成的异质结构中畴间对比的起源。在电子束正常入射下,在亮场显微镜模式下观察到这种对比。该异质结构由生长在W(110)表面的两畴α相锑烯上的单畴β相组成。我们发现这种对比是由于形成了两种不同的摩尔超晶格,它直接反映了α锑烯的双畴结构。我们还证明了对比取决于两种莫尔条纹的相对对称性和晶体学。
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引用次数: 0
Approaching one nanosecond temporal resolution with square-wave-based control signals for interference gating 接近一纳秒的时间分辨率的方波控制信号干扰门控
IF 2.1 3区 工程技术 Q2 MICROSCOPY Pub Date : 2025-07-21 DOI: 10.1016/j.ultramic.2025.114208
Simon Gaebel , Hüseyin Çelik , Dirk Berger , Christoph T. Koch , Michael Lehmann , Tolga Wagner
Interference gating (iGate) has emerged as a valuable and instrumentally easy-to-implement technique for time-resolved electron holography, allowing the study of dynamic processes on the nanosecond scale. Traditionally, iGate has relied on noise-based control signals, which, while effective, present challenges in achieving high repetition rates due to the complexity of signal generation and transmission. In this work, a square-wave-based control signal for iGate is introduced, offering a simpler and more robust alternative. Experimental validation indicates that this approach maintains comparable performance to the noise-based signal while enabling an order-of-magnitude improvement in temporal resolution, reaching 1.9ns with our current instrumentation. This advancement holds promise for improved time-resolved investigations of ultrafast nanoscale phenomena in TEM, providing a low barrier to entry.
干涉门控(iGate)已经成为一种有价值且易于实现的时间分辨电子全息技术,允许在纳秒尺度上研究动态过程。传统上,iGate依赖于基于噪声的控制信号,虽然有效,但由于信号产生和传输的复杂性,在实现高重复率方面存在挑战。在这项工作中,引入了一种基于方波的iGate控制信号,提供了一种更简单、更鲁棒的替代方案。实验验证表明,该方法保持了与基于噪声的信号相当的性能,同时在时间分辨率上实现了数量级的提高,使用我们目前的仪器达到1.9ns。这一进展有望改善TEM中超快纳米级现象的时间分辨研究,提供低进入门槛。
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引用次数: 0
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Ultramicroscopy
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