Scanning electron microscopy imaging of dislocations in bulk materials, using electron channeling contrast

The imaging and characterization of dislocations is commonly carried out by thin foil transmission electron microscopy (TEM) using diffraction contrast imaging. However, the thin foil approach is limited by difficult sample preparation, thin foil artifacts, relatively small viewable areas, and constraints on carrying out in situ studies. Electron channeling imaging of electron channeling contrast imaging (ECCI) offers an alternative approach for imaging crystalline defects, including dislocations. Because ECCI is carried out with field emission gun scanning electron microscope (FEG-SEM) using bulk specimens, many of the limitations of TEM thin foil analysis are overcome. This paper outlines the development of electron channeling patterns and channeling imaging to the current state of the art. The experimental parameters and set up necessary to carry out routine channeling imaging are reviewed. A number of examples that illustrate some of the advantages of ECCI over thin foil TEM are presented along with a discussion of some of the limitations on carrying out channeling contrast analysis of defect structures.     

Energy dispersive spectroscopy analysis of aluminium segregation in silicon carbide grain boundaries

The aluminium distribution in polycrystalline SiC hot‐pressed with aluminium, boron and carbon additives was studied using X‐ray energy‐dispersive spectroscopy (EDS) and transmission electron microscopy (TEM). The Al excess in homophase SiC grain boundary films was determined, taking into account dissolved Al in the SiC lattice. In the spot‐EDS analysis, an electron beam probe with a calibrated diameter was formed, and the total beam–specimen interaction volume was defined, taking the beam spreading through crystalline TEM foil into consideration. EDS spectra were collected from regions containing intergranular films and adjacent matrix grains, respectively. A theoretical treatment was presented and experimental errors were estimated, with a further discussion about the effects of foil thickness. Experimental examples are given, followed by statistical EDS analyses for grain boundary films in SiC samples hot‐pressed with increased amounts of Al additions. The results demonstrated a substantial Al segregation in the nanometer‐wide intergranular films in all samples. Al additions higher than 3 wt% saturated the Al concentrations in SiC grains and in grain boundary films. The effect of foil thickness, and the parameters for determining the optimum incident beam diameter in the EDS analysis are discussed.     

Orientation and phase mapping in the transmission electron microscope using precession‐assisted diffraction spot recognition: state‐of‐the‐art results

A recently developed technique based on the transmission electron microscope, which makes use of electron beam precession together with spot diffraction pattern recognition now offers the possibility to acquire reliable orientation/phase maps with a spatial resolution down to 2 nm on a field emission gun transmission electron microscope. The technique may be described as precession‐assisted crystal orientation mapping in the transmission electron microscope, precession‐assisted crystal orientation mapping technique–transmission electron microscope, also known by its product name, ASTAR, and consists in scanning the precessed electron beam in nanoprobe mode over the specimen area, thus producing a collection of precession electron diffraction spot patterns, to be thereafter indexed automatically through template matching. We present a review on several application examples relative to the characterization of microstructure/microtexture of nanocrystalline metals, ceramics, nanoparticles, minerals and organics. The strengths and limitations of the technique are also discussed using several application examples.     

Images obtained in STEM of gold particles condensed on the top of thick single crystals of copper

It is proposed that when a thin sample is mounted on the top surface of a thick single crystal foil, this foil may function as a collector aperture with regard to the radiation transmitted through the thin sample. The detailed aspects of how the crystal foil may perform as an aperture are discussed in terms of the electron equivalent of the Borrmann effect in crystals. Experiments are presented which demonstrate that the image of the thin sample is sensitive to the thickness of the single crystal foil and to its orientation with regard to the beam axis. It is concluded from the experimental results that the crystal foil does perform a collector aperture-like function.     

Evidence of multimicrometric coherent γ′ precipitates in a hot‐forged γ–γ′ nickel‐based superalloy

This paper demonstrates the existence of large γ’ precipitates (several micrometres in diameter) that are coherent with their surrounding matrix grain in a commercial γ–γ’ nickel‐based superalloy. The use of combined energy dispersive X‐ray spectrometry and electron backscattered diffraction (EBSD) analyses allowed for revealing that surprising feature, which was then confirmed by transmission electron microscopy (TEM). Coherency for such large second‐phase particles is supported by a very low crystal lattice misfit between the two phases, which was confirmed thanks to X‐ray diffractograms and TEM selected area electron diffraction patterns. Dynamic recrystallization of polycrystalline γ–γ’ nickel‐based superalloys has been extensively studied in terms of mechanisms and kinetics. As in many materials with low stacking fault energy, under forging conditions, the main softening mechanism is discontinuous dynamic recrystallization. This mechanism occurs with preferential nucleation on the grain boundaries of the deformed matrix. The latter is then being consumed by the growth of the newly formed grains of low energy and by nucleation that keeps generating new grains. In the case of sub‐solvus forging, large γ’ particles usually pin the migrating boundaries and thus limit grain growth to a size which is determined by the distribution of second‐phase particles, in good agreement with the Smith–Zener model. Under particular circumstances, the driving force associated with the difference in stored energy between the growing grains and the matrix can be large enough that the pinning forces can be overcome, and some grains can then reach much larger grain sizes. In the latter exceptional case, some intragranular primary γ’ particles can be observed, although they are almost exclusively located on grain boundaries and triple junctions otherwise. In both cases, primary precipitates have no special orientation relationship with the surrounding matrix grain(s). This paper demonstrates the existence of high fractions of large γ’ precipitate (several micrometres in diameter) that are coherent with their surrounding matrix grain, in a commercial γ–γ’ nickel‐based superalloy. Such a configuration is very surprising, because there is apparently no reason for the coherency of such particles.     

Synergistic effects of anisotropy and image force on TEM diffraction contrast of dislocation loops

Based on column approximation (CA) assumption, many-beam Schaeublin–Stadelmann diffraction equations are employed for simulating the transmission electron microscopy (TEM) diffraction image contrast of dislocation loops within thin TEM foil of finite thickness, and two beam and many beam diffraction conditions are compared. Moreover, the effects of materials anisotropy and free surface relaxation induced elastic fields distortion of dislocation loops on the black-white image contrast are specially focused. It is found that anisotropy has a remarkable impact on the TEM image contrast of dislocation loop, and free surface relaxation induced image forces can change the black-white contrast features when dislocation loops are near TEM foil free surfaces. Thus, in order to make reliable judgment on the nature of defects, effects of free surface and anisotropy should be included when analysing irradiation induced dislocation loops and other type of defects in in-situ electron, proton, heavy-ion irradiation experiments under TEM environments.     

Polycrystal orientation maps from TEM

Determination of topography of crystallite orientations is an important technique of investigation of polycrystalline materials. A system for creating orientation maps using transmission electron microscope (TEM) Kikuchi patterns and Convergent beam electron diffraction patterns is presented. The orientation maps are obtained using a step-by-step beam scan on a computer-controlled TEM equipped with a CCD camera. At each step, acquired diffraction patterns are indexed and orientations are determined. Although, the approach used is similar to that applied in SEM/electron back scattered diffraction (EBSD) orientation imaging setups, the TEM-based system considerably differs from its SEM counterpart. The main differences appear due to specific features of TEM and SEM diffraction patterns. Also, the resulting maps are not equivalent. On these generated by TEM, the accuracy of orientation determination can be better than 0.1 degrees. The spatial resolution is estimated to be about 10nm. The latter feature makes the TEM orientation mapping system an important tool for studies at fine scale unreachable by SEM/EBSD systems. The automatic orientation mapping is expected to be a useful complement of the conventional TEM contrast images. The new technique will be essential for characterization of fine structure materials. To illustrate that, example maps of an aluminum sample produced by severe plastic deformation are included.     

Dynamical electron diffraction simulation for non‐orthogonal crystal system by a revised real space method

In the transmission electron microscopy, a revised real space (RRS) method has been confirmed to be a more accurate dynamical electron diffraction simulation method for low‐energy electron diffraction than the conventional multislice method (CMS). However, the RRS method can be only used to calculate the dynamical electron diffraction of orthogonal crystal system. In this work, the expression of the RRS method for non‐orthogonal crystal system is derived. By taking Na₂Ti₃O₇ and Si as examples, the correctness of the derived RRS formula for non‐orthogonal crystal system is confirmed by testing the coincidence of numerical results of both sides of Schrödinger equation; moreover, the difference between the RRS method and the CMS for non‐orthogonal crystal system is compared at the accelerating voltage range from 40 to 10 kV. Our results show that the CMS method is almost the same as the RRS method for the accelerating voltage above 40 kV. However, when the accelerating voltage is further lowered to 20 kV or below, the CMS method introduces significant errors, not only for the higher‐order Laue zone diffractions, but also for zero‐order Laue zone. These indicate that the RRS method for non‐orthogonal crystal system is necessary to be used for more accurate dynamical simulation when the accelerating voltage is low. Furthermore, the reason for the increase of differences between those diffraction patterns calculated by the RRS method and the CMS method with the decrease of the accelerating voltage is discussed.     

Static-charging mitigation and contamination avoidance by selective carbon coating of TEM samples

Prior to transmission electron microscopy (TEM) analyses, insulating specimens need to become coated with a charge-draining layer. Rather than coating the entire TEM foil with a thin film of homogeneous thickness, selective coating is proposed. Using a novel preparation tool, peripheral parts of the sample are coated with a relatively thick (4-8 nm) carbon film while the central, electron-transparent part of the sample is hidden behind a shape-adopted mask and thus not directly exposed to carbon deposition. Beneath the mask, an ultrathin (3-7 A) carbon film is formed that is (i) thick enough to drain charges evolving upon electron irradiation in the electron microscope and (ii) thin enough to avoid typical contamination effects caused by superficial carbon diffusion. Consequently, image quality is becoming enhanced in high-resolution imaging and sensitivity is significantly increased in all nano-beam related techniques including elemental analytics, convergent-beam and nano-beam electron diffraction, and spectral imaging.     

EBSD and TEM investigation of the hot deformation substructure characteristics of a type 316L austenitic stainless steel

The evolution of crystallographic texture and deformation substructure was studied in a type 316L austenitic stainless steel, deformed in rolling at 900 °C to true strain levels of about 0.3 and 0.7. Electron backscatter diffraction (EBSD) and transmission electron microscopy (TEM) were used in the investigation and a comparison of the substructural characteristics obtained by these techniques was made. At the lower strain level, the deformation substructure observed by EBSD appeared to be rather poorly developed. There was considerable evidence of a rotation of the pre‐existing twin boundaries from their original orientation relationship, as well as the formation of highly distorted grain boundary regions. In TEM, at this strain level, the substructure was more clearly revealed, although it appeared rather inhomogeneously developed from grain to grain. The subgrains were frequently elongated and their boundaries often approximated to traces of {111} slip planes. The corresponding misorientations were small and largely displayed a non‐cumulative character. At the larger strain, the substructure within most grains became well developed and the corresponding misorientations increased. This resulted in better detection of sub‐boundaries by EBSD, although the percentage of indexing slightly decreased. TEM revealed splitting of some sub‐boundaries to form fine microbands, as well as the localized formation of microshear bands. The substructural characteristics observed by EBSD, in particular at the larger strain, generally appeared to compare well with those obtained using TEM. With increased strain level, the mean subgrain size became finer, the corresponding mean misorientation angle increased and both these characteristics became less dependent on a particular grain orientation. The statistically representative data obtained will assist in the development of physically based models of microstructural evolution during thermomechanical processing of austenitic stainless steels.     

Precession electron diffraction‐assisted crystal phase mapping of metastable c‐GaN films grown on (001) GaAs

The control growth of the cubic meta‐stable nitride phase is a challenge because of the crystalline nature of the nitrides to grow in the hexagonal phase, and accurately identifying the phases and crystal orientations in local areas of the nitride semiconductor films is important for device applications. In this study, we obtained phase and orientation maps of a metastable cubic GaN thin film using precession electron diffraction (PED) under scanning mode with a point‐to‐point 1 nm probe size beam. The phase maps revealed a cubic GaN thin film with hexagonal GaN inclusions of columnar shape. The orientation maps showed that the inclusions have nucleation sites at the cubic GaN {111} facets. Different growth orientations of the inclusions were observed due to the possibility of the hexagonal {0001} plane to grow on any different {111} cubic facet. However, the generation of the hexagonal GaN inclusions is not always due to a 60° rotation of a {111} plane. These findings show the advantage of using PED along with phase and orientation mapping, and the analysis can be extended to differently composed semiconductor thin films. Microsc. Res. Tech. 77:980–985, 2014. © 2014 Wiley Periodicals, Inc.     

CBED and LACBED characterization of crystal defects

Convergent‐beam electron diffraction (CBED) obtained with a focused incident beam is well known for the identification of the point and space groups but it can also be used for the analysis of stacking faults and antiphase boundaries. Large‐angle convergent‐beam electron diffraction (LACBED) is performed with a large defocused incident beam and is well adapted to the characterization of most types of crystal defects: point defects, perfect and partial dislocations, stacking faults, antiphase boundaries and grain boundaries. Among the advantages of these methods with respect to the conventional transmission electron microscopy methods, are that one or few patterns are required for a full analysis and the interpretations are easy and unambiguous. The LACBED technique is particularly useful for the analysis of dislocations present in anisotropic and beam‐sensitive materials.     

电子束蒸发沉积碲锗铅薄膜的微结构和化学组分研究

为了探寻碲锗铅(Pb_(1-x)Ge_xTe)薄膜的最佳沉积方式,在硅基片上采用电子束蒸发沉积碲锗铅(Pb_(0.78)Ge_(0.22)Te)薄膜。使用X射线衍射(XRD)、电子扫描显微镜(SEM)、能量散射X射线分析(EDAX)等手段对薄膜的微结构和化学配比特性进行了分析。发现碲锗铅薄膜为多晶结构,具有明显的择优取向,晶粒多为矩形,薄膜中未出现其它相关氧化物。与热蒸发膜层相比,电子束蒸发沉积的膜层有更为完善的晶体结构。     

Influence of substrate orientation on the morphologyand orientation of LaNiO3 thin films

LaNiO₃ thin films were successfully prepared by a chemical method from citrate precursors. The LNO precursor solution was spin‐coated onto Si (100) and Si (111) substrates. To obtain epitaxial or highly oriented films, the deposited layers were slowly heated in a gradient thermal field, with a heating rate of 1° min^?1, and annealed at 700°C. The influence of different substrate orientations on the thin film morphology was investigated using atomic force microscopy and X‐ray diffraction analysis. Well‐crystallized films with grains aligned along a certain direction were obtained on both substrates. Films deposited on both substrates were very smooth, but with a different grain size and shape depending on the crystal orientation. Films deposited on Si (100) grew in the (110) direction and had elongated grains, whereas those on Si (111) grew in the (211) direction and had a quasi‐square grain shape.     

TEM foil preparation of sub-micrometre sized individual grains by focused ion beam technique

Analysis of presolar silicate grains provides new knowledge on interstellar and circumstellar environments and can be used to test models of the Galactic chemical evolution. However, structural information of these grains is rare because sample preparation for transmission electron microscopy is very difficult due to the small dimensions of these grains (<0.5 μm). With the use of the focused ion beam technique thin foils from these grains for transmission electron microscopy analysis can be prepared. Nevertheless, reaching the required precision of some tens of nanometres for the preparation of the transmission electron microscopy foil in the place of interest is not trivial. Furthermore, in the current samples, the grain of interest can only be identified by its different isotopic composition; i.e. there is no contrast difference in scanning electron microscopy or transmission electron microscopy images which allow the identification of the grain. Therefore, the grain has to be marked in some way before preparing the transmission electron microscopy foil. In the present paper, a method for transmission electron microscopy foil preparation of grains about 200 to 400 nm in diameter is presented. The method utilizes marking of the grain by Pt deposition and milling of holes to aid in the exact orientation of the transmission electron microscopy foil with respect to the grain. The proposed method will be explained in detail by using an example grain.     

Effect of sample bending on diffracted intensities observed in CBED patterns of plan view strained samples

Convergent beam electron diffraction is used to study the effect of the sample bending on diffracted intensities as observed in transmission electron microscopy (TEM). Studied samples are made of thin strained semiconductor Ga(1-)(x)In(x)As epitaxial layers grown on a GaAs substrate and observed in plan view. Strong variations of the diffracted intensities are observed depending on the thinning process used for TEM foil preparation. For chemically thinned samples, strong bending of the substrate occurs, inducing modifications of both kinematical and dynamical Bragg lines. For mechanically thinned samples, bending of the substrate is negligible. Kinematical lines are unaffected whereas dynamical lines have slightly asymmetric intensities. We analyse these effects using finite element modelling to calculate the sample strain coupled with dynamical multibeam simulations for calculating the diffracted intensities. Our results correctly reproduce the qualitative features of experimental patterns, clearly demonstrating that inhomogeneous displacement fields along the electron beam within the substrate are responsible for the observed intensity modifications.     

Diffraction effects and inelastic electron transport in angle‐resolved microscopic imaging applications

We analyse the signal formation process for scanning electron microscopic imaging applications on crystalline specimens. In accordance with previous investigations, we find nontrivial effects of incident beam diffraction on the backscattered electron distribution in energy and momentum. Specifically, incident beam diffraction causes angular changes of the backscattered electron distribution which we identify as the dominant mechanism underlying pseudocolour orientation imaging using multiple, angle‐resolving detectors. Consequently, diffraction effects of the incident beam and their impact on the subsequent coherent and incoherent electron transport need to be taken into account for an in‐depth theoretical modelling of the energy‐ and momentum distribution of electrons backscattered from crystalline sample regions. Our findings have implications for the level of theoretical detail that can be necessary for the interpretation of complex imaging modalities such as electron channelling contrast imaging (ECCI) of defects in crystals. If the solid angle of detection is limited to specific regions of the backscattered electron momentum distribution, the image contrast that is observed in ECCI and similar applications can be strongly affected by incident beam diffraction and topographic effects from the sample surface. As an application, we demonstrate characteristic changes in the resulting images if different properties of the backscattered electron distribution are used for the analysis of a GaN thin film sample containing dislocations.     

Using EBSD and TEM-Kikuchi patterns to study local crystallography at the domain boundaries of lead zirconate titanate

Reliable EBSD mapping of 90° domains in a tetragonal ferroelectric perovskite has been achieved for the first time, together with reliable automated orientation determination from TEM‐Kikuchi patterns. This has been used to determine misorientation angles at 90° domain boundaries and thus local c/a ratios. The sources of orientation noise/error and their effects on the misorientation angle data have been thoroughly analyzed and it is found that this gives a cosine distribution of misorientation angles about the mean with a characteristic width related to the width of the orientation noise distribution. In most cases, a good agreement is found between local c/a ratios and global measurements by X‐ray diffraction, but some clear discrepancies have also been found suggesting that real local variations are present, perhaps as a consequence of compositional inhomogeneities.     

On the interpretation of the forbidden spots observed in the electron diffraction patterns of flat Au triangular nanoparticles

In many cases nanostructures present forbidden spots in their electron diffraction patterns when they are observed by transmission electron microscopy (TEM). To interpret their TEM and high resolution transmission electron microscopy (HRTEM) images properly, an understanding of the origin of these spots is necessary. In this work we comment on the origin of the forbidden spots observed in the [111] and [112] electron diffraction patterns of flat gold triangular nanoparticles. The forbidden spots were successfully indexed as corresponding to the first laue Zone (FOLZ) and the HRTEM images presented a contrast produced by the interference of the zero-order Laue zone (ZOLZ) and FOLZ spots. We discuss the use of the forbidden spots in the study of the structure of nanoparticles and show that they are related to the shape and incompleteness of layers in the very thin particles.     

Characterization of nitride thin films by electron backscatter diffraction

Thin films incorporating GaN, InGaN and AlGaN are presently arousing considerable excitement because of their suitability for UV and visible light‐emitting diodes and laser diodes. However, because of the lattice mismatch between presently used substrates and epitaxial nitride thin films, the films are of variable quality. In this paper we describe our preliminary studies of nitride thin films using electron backscattered diffraction (EBSD). We show that the EBSD technique may be used to reveal the relative orientation of an epitaxial thin film with respect to its substrate (a 90° rotation between a GaN epitaxial thin film and its sapphire substrate is observed) and to determine its tilt (a GaN thin film was found to be tilted by 13 ± 1° towards [101 0]_GaN), where the tilt is due to the inclination of the sapphire substrate (cut off‐axis by 10° from (0001)_sapphire towards (101 0)_sapphire). We compare EBSD patterns obtained from As‐doped GaN films grown by plasma‐assisted molecular beam epitaxy (PA‐MBE) with low and high As₄ flux, respectively. Higher As₄ flux results in sharper, better defined patterns, this observation is consistent with the improved surface morphology observed in AFM studies. Finally, we show that more detail can be discerned in EBSD patterns from GaN thin films when samples are cooled.