Development of a technique for high resolution electron microscopic observation of nano-materials at elevated temperatures

A technique for high resolution transmission electron microscopic (TEM) observation of nano-materials at very high temperatures has been developed. A spirally wound tungsten wire, normally used as the heating element of a high resolution-high temperature-specimen heating holder, was coated with a thin carbon film and the carbon film was used as the substrate of nanometer-sized specimen. The carbon film was securely self-adhered on the heater and the form of the carbon film remained unchanged until the tungsten heater is heated to around 1173 K. Temperature distribution on the carbon film has been measured by observing the sublimation of ZnS particles. Behavior of gold atoms on a surface of gold nano-particles dispersed on the carbon film has been clearly observed at 773 K in a scanning transmission electron microscope (STEM).     

A specimen-drift-free EDX mapping system in a STEM for observing two-dimensional profiles of low dose elements in fine semiconductor devices

We developed a specimen-drift-free energy-dispersive X-ray (EDX) mapping system in a scanning transmission electron microscope (STEM) to improve the sensitivity and spatial resolution of EDX elemental mapping images. The amount of specimen drift was analysed from two STEM images before and after specimen drift by using the phase-correlation method, and was compensated for with an image-shift deflector of the STEM by the displacement of the scanning electron beam. We applied this system to observe the two-dimensional distribution of low dose arsenic in silicon semiconductor devices. The sensitivity of the elemental mapping was improved to several tenths atomic % for arsenic atoms while maintaining a spatial resolution of 2 nm.     

The development and characteristics of a high-speed EELS mapping system for a dedicated STEM

A new EELS (electron energy loss spectroscopy) real-time elemental mapping system has been developed for a dedicated scanning transmission electron microscope (STEM). The previous two-window-based jump-ratio system has been improved by a three-window-based system. It is shown here that the three-window imaging method has less artificial intensity in elemental maps than the two-window-based method. Using the new three-window system, the dependence of spatial resolution on the energy window width was studied experimentally and also compared with TEM-based EELS. Here it is shown experimentally that the spatial resolution of STEM-based EELS is independent of the energy window width in a range from 10 eV to 60 eV.     

New views of materials through aberration-corrected scanning transmission electron microscopy

The successful correction of third-order and, more recently, fifth-order aberrations has enormously enhanced the capabilities of the scanning transmission electron microscope (STEM), by not only achieving record resolution, but also allowing near 100% efficiency for electron energy loss spectroscopy, and higher currents for two-dimensional spectrum imaging. These advances have meant that the intrinsic advantages of the STEM, incoherent imaging and simultaneous collection of multiple complementary images can now give new insights into many areas of materials physics. Here, we review a number of examples, mostly from the field of complex oxides, and look towards new directions for the future.     

Application of Aberration-Corrected TEM and Image Simulation to Nanoelectronics and Nanotechnology

The image quality in electron microscopy often suffers from lens aberration. As a result of lens aberrations, critical information appears distorted at the atomic scale in high-resolution transmission electron microscopy (HRTEM). In scanning TEM (STEM), the spatial resolution of images and the quality of spectroscopic data are greatly reduced. With the recent introduction of aberration-corrected lenses and monochromators, new and exciting images with sub-0.1-nm spatial resolution are now recorded routinely, and electron energy loss data has been used to determine the location of a single atom in an atomic column. As a result of the decreased focal depth of an aberration-corrected lens used in STEM, the dream of three-dimensional (3-D) atomic resolution is one step closer and for HRTEM it was shown that 3-D imaging with atomic resolution is feasible. However, understanding imaging and spectroscopy in HRTEM and STEM still requires refined modeling of the underlying electron scattering processes by multislice image simulation. Since research into the physics and technology of nanoelectronic devices has already moved into sub-10-nm transistor gate lengths, the need for well-understood imaging and spectroscopy at nanoscale dimensions is already upon us. Fortunately, nanowires and other nanotechnology materials serve as useful test samples as well as being potential materials for future nanoelectronics. This enables early development of microscopy methods that will be used to investigate future generations of integrated circuits     

Prospects of atomic resolution imaging with an aberration-corrected STEM

We investigated high-resolution scanning transmission electron microscope (STEM) images obtained from a microscope equipped with a spherical aberration corrector. The probe size (full-width at half-maximum) is reduced to 0.76 A at 200 kV by assuming the fifth-order spherical aberration coefficient C5 = 100 mm. For the simulation we have used the recently developed scheme for a STEM image simulation based on the Fast Fourier Transform (FFT) multislice algorithm. The peak-to-background (P/B) ratio of the high-angle annular dark-field (HAADF) image is significantly improved at a thin specimen region. Although the P/B ratio becomes worse at a thicker region, the resolution is kept high even at such a region. An almost true HAADF signal will be obtained even from a weak-scattering phosphorous column in InP [001] when the background is subtracted. In the bright-field image the coherent character of elastic scattering is suppressed by averaging over a large convergence angle, making the specimen effectively self-luminous. The claim that HAADF imaging is relatively insensitive to a defocus as well as a specimen thickness is valid only qualitatively, and a detailed image simulation will be required for a quantitative analysis as in the case of the conventional transmission electron microscope. It was noted that the delta function approximation for the object function may not be applicable for a very fine probe, and that the achievable resolution of the HAADF imaging will be limited by the widths of the high-angle thermal diffuse scattering potential.     

Scanning transmission electron microscopy and its application to the study of nanoparticles and nanoparticle systems

Scanning transmission electron microscopy (STEM) techniques can provide imaging, diffraction and spectroscopic information, either simultaneously or in a serial manner, of the specimen with an atomic or a sub-nanometer spatial resolution. High-resolution STEM imaging, when combined with nanodiffraction, atomic resolution electron energy-loss spectroscopy and nanometer resolution X-ray energy dispersive spectroscopy techniques, is critical to the fundamental studies of importance to nanoscience and nanotechnology. The availability of sub-nanometer or sub-angstrom electron probes in a STEM instrument, due to the use of a field emission gun and aberration correctors, ensures the greatest capabilities for studies of sizes, shapes, defects, crystal and surface structures, and compositions and electronic states of nanometer-size regions of thin films, nanoparticles and nanoparticle systems. The various imaging, diffraction and spectroscopy modes available in a dedicated STEM or a field emission TEM/STEM instrument are reviewed and the application of these techniques to the study of nanoparticles and nanostructured catalysts is used as an example to illustrate the critical role of the various STEM techniques in nanotechnology and nanoscience research.     

Progress in aberration-corrected scanning transmission electron microscopy

A new corrector of spherical aberration (C(S)) for a dedicated scanning transmission electron microscope (STEM) is described and its results are presented. The corrector uses strong octupoles and increases C(C) by only 0.2 mm relative to the uncorrected microscope. Its overall stability is greatly improved compared to our previous design. It has achieved a point-to-point resolution of 1.23 A in high-angle annular dark field images at 100 kV. It has also increased the current available in a 1.3 A-sized probe by about a factor of ten compared to existing STEMs. Its operation is greatly assisted by newly developed autotuning software which measures all the aberration coefficients up to fifth order in less than one minute. We conclude by discussing the present limits of aberration-corrected STEM, and likely future developments.     

单晶硅表面STM成像理论模型与实验分析

结合扫描隧道显微镜(STM)成像实验和第一性原理原子级模拟计算的方法已经成为材料界面表征的重要手段。超高真空条件下的STM可用于直接观察单原子等微观结构,但其成像原理还未被理解清楚。STM扫描测得的试件表面原子级图像并不直接反映材料原子的形态,实际上是表面形貌和表面电子态局域密度的综合结果。为了解释STM成像,采用第一性原理Siesta方法,研究了Si(001)面STM成像过程的电子结构,对表面粒子的原子轨道和相应的电荷密度进行计算。讨论了等高模式下扫描高度对局域电子云密度分布的影响,并分析了STM针尖几何形状对模拟结果的影响。研究表明,材料表面原子的电子云密度分布可以用来解释STM成像精度和扫描高度对比的变化。     

Atomic resolution Z-contrast imaging of semiconductors

The direct interpretability of atomic resolution Z-contrast images obtained from a scanning transmission electron microscope (STEM) makes this imaging technique particularly powerful for the analysis of interfaces and defects in semiconductor materials and devices. In this paper, the principles of the technique are outlined and representative examples of its use are presented. In particular, we show the use of Z-contrast imaging to determine the polarity of a CdTe film grown on a Si substrate, the atomic structures of stacking faults and threading dislocation cores in GaN, and the atomistic structure of an ohmic metal/semiconductor contact of Au/GaAs.     

HRTEM imaging of atoms at sub-Angström resolution

John Cowley and his group at Arizona State University pioneered the use of transmission electron microscopy for high-resolution imaging. Images were achieved three decades ago showing the crystal unit cell content at better than 4 A resolution. This achievement enabled researchers to pinpoint the positions of heavy atom columns within the unit cell. Lighter atoms appear as resolution is improved to sub-Angstr?m levels. Currently, advanced microscopes can image the columns of the light atoms (carbon, oxygen, nitrogen) that are present in many complex structures, and even the lithium atoms present in some battery materials. Sub-Angstr?m imaging, initially achieved by focal-series reconstruction of the specimen exit surface wave, will become commonplace for next-generation electron microscopes with C(S)-corrected lenses and monochromated electron beams. Resolution can be quantified in terms of peak separation and inter-peak minimum, but the limits imposed on the attainable resolution by the properties of the microscope specimen need to be considered. At extreme resolution the 'size' of atoms can mean that they will not be resolved even when spaced farther apart than the resolution of the microscope.     

Development of a 1 MV field-emission transmission electron microscope

We developed a 1 MV field-emission transmission electron microscope. This paper reports details and specifications of the instrument. The microscope was designed to obtain a bright and coherent electron beam by using the field emission gun equipped with a pre-accelerating magnetic lens and the high-voltage power supply with high stability (0.5 ppm min(-1)). Using this microscope, the brightness of 1.8 x 10(10) A cm(-2) sr(-1) and the lattice resolution of 49.8 pm were attained.     

From electron energy-loss spectroscopy to multi-dimensional and multi-signal electron microscopy

This review intends to illustrate how electron energy-loss spectroscopy (EELS) techniques in the electron microscope column have evolved over the past 60 years. Beginning as a physicist tool to measure basic excitations in solid thin foils, EELS techniques have gradually become essential for analytical purposes, nowadays pushed to the identification of individual atoms and their bonding states. The intimate combination of highly performing techniques with quite efficient computational tools for data processing and ab initio modeling has opened the way to a broad range of novel imaging modes with potential impact on many different fields. The combination of Angstr?m-level spatial resolution with an energy resolution down to a few tenths of an electron volt in the core-loss spectral domain has paved the way to atomic-resolved elemental and bonding maps across interfaces and nanostructures. In the low-energy range, improved energy resolution has been quite efficient in recording surface plasmon maps and from them electromagnetic maps across the visible electron microscopy (EM) domain, thus bringing a new view to nanophotonics studies. Recently, spectrum imaging of the emitted photons under the primary electron beam and the spectacular introduction of time-resolved techniques down to the femtosecond time domain, have become innovative keys for the development and use of a brand new multi-dimensional and multi-signal electron microscopy.     

Application of atomic scale STEM techniques to the study of interfaces and defects in materials

Incoherent imaging and analysis techniques in the scanning transmission electron microscope (STEM) provide the potential to map changes in structure, composition and bonding that occur at materials interfaces and defects on the fundamental atomic scale. Such comprehensive characterization capabilities permit a detailed analysis of the structure-property relationships of interfaces and defects to be performed. In this paper, we discuss the resolution limits of such techniques in the JEOL 2010F STEM/TEM operating both under standard conditions and at elevated temperatures. Examples of the use of such techniques to quantify the atomic scale defect chemistry at interfaces and defects in perovskite oxides, the growth and structure of II-VI and III-V quantum dots and the electronic structure of threading dislocations in GaN will also be presented.     

Microstructure of Heteroepitaxial ZnTe Grown on GaAs(211)B by Molecular Beam Epitaxy

ZnTe was grown on GaAs(211)B by molecular beam epitaxy (MBE). Structural properties and strain relaxation at the ZnTe/GaAs(211)B interface were investigated by high resolution transmission electron microscopy (HRTEM) and scanning transmission electron microscopy (STEM). Application of digital image processing involving a filtered inverse fast Fourier transformation revealed an array of misfit dislocations at the interface and allowed strain relaxation to be estimated. Only one twin defect was observed in the HRTEM images, and details of this twin defect were investigated by STEM.     

Atomically resolved mapping of EELS fine structures

Over the past two or three decades, nanoscience and nanotechnology have clearly established themselves as prominent domains in research in physics, not only because of the innovative concepts and properties that they display but also for their capacity to generate many important applications and commercial developments. As many of these new devices exhibit a range of properties (transport, optical, magnetic, catalysis) which are governed by local structural and electronic configurations, such as coordination and bonding at the atomic level, it is no surprise that new tools of investigation are constantly being developed for imaging, analyzing, understanding and controlling at the relevant scale. Among them, electron microscopy has recently demonstrated its ability to meet many of these requirements. In particular, Å-sized probes are nowadays generated by aberration correctors in a scanning transmission electron microscope (STEM) and they can investigate the electron excitation spectrum of the specimen (through electron energy-loss spectroscopy, EELS) with a typical energy resolution of 0.1–0.3 eV over a broad spectral band from the IR to the X ray domain. In the high energy range, characteristic signals due to the excitation of atomic core levels are quite useful because they identify the atoms in the analyzed volume (which can itself be as small as a single atom) and can therefore deliver atomically-resolved elemental maps. But the pixel-by-pixel recording of the fine structures beyond the characteristic threshold is much more informative and tells us how the excited atom is surrounded by its neighbors, what is its exact structural environment and its charge population. The present review focuses on this particularly exciting field, with a special interest in the types of information accessible and their signature. After summarizing the ingredients required for successful experiments (instrumental as well as theoretical), examples encountered in different situations, in particular in single layers of 2D materials and at the interfaces in oxide heterostructures, will demonstrate the present capabilities of this STEM-EELS technique.     

Atomic‐Scale Visualization of Polarization Pinning and Relaxation at Coherent BiFeO3/LaAlO3 Interfaces

Complex oxide heterointerfaces, which play host to an incredible variety of interface physical phenomena, are of great current interest in introducing new functionalities to systems. Here, coherent super‐tetragonal BiFeO₃/LaAlO₃ and rhombohedral BiFeO₃/LaAlO₃ heterointerfaces are investigated by using a combination of high‐angle annular dark‐field (HAADF) imaging and annular bright‐field (ABF) imaging in a spherical aberration (Cs) corrected scanning transmission electron microscope (STEM), and first‐principles calculations. The complicated ferroelectric polarization pinning and relaxation that occurs at both interfaces is revealed with atomic resolution, with a dramatic change in structure of BiFeO₃, from cubic to super‐tetragonal‐like. The results enable a detailed explanation to be given of how non‐bulk phase structures are stabilized in thin films of this material.     

利用场发射扫描电镜的低电压高性能进行材料表征

场发射扫描电子显微镜（FESEM）是一种高分辨扫描电镜,在材料分析中得到广泛应用。尤其是良好的低压高空间分辨性能和低压下良好的SE像相互结合使用,使SEM应用范围得到扩展。     

STEM role in failure analysis

The STEM is a technique used in failure analysis that solves the gap between conventional Scanning Electron Microscope (SEM) and Transmission Electron Microscope (TEM) and enables the acquisition of high resolution images of a sample mounted on a TEM grid. This paper explains the theory of STEM imaging and presents its application through some failure analysis works preformed with a FEI Strata Dual Beam 235 mounted with a STEM detector and an EDAX Energy dispersive X-ray detector.This technique is essentially used for failure root cause research and is particularly interesting when combined with elemental analysis, as it gives high resolution results when performed on thin samples.