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Electron diffraction

Electron diffraction is a generic term for phenomena associated with changes in the direction of electron beams due to elastic interactions with atoms. It occurs due to elastic scattering, when there is no change in the energy of the electrons. The negatively charged electrons are scattered due to Coulomb forces when they interact with both the positively charged atomic core and the negatively charged electrons around the atoms. The resulting map of the directions of the electrons far from the sample is called a diffraction pattern, see for instance Figure 1. Beyond patterns showing the directions of electrons, electron diffraction also plays a major role in the contrast of images in electron microscopes.

A primer on electron diffraction
All matter can be thought of as matter waves, and a classic example is the Young's two-slit experiment shown in Figure 2, where a wave impinges upon two slits in the first of the two images (blue waves). After going through the slits there are directions where the wave is stronger, ones where it is weaker – the wave has been diffracted. If instead of two slits there are a number of small points then similar phenomena can occur as shown in the second image where the wave (red and blue) is coming in from the bottom right corner. This is comparable to diffraction of an electron wave where the small dots would be atoms in a small crystal, see also note. Note the strong dependence on the relative orientation of the crystal and the incoming wave. Close to an aperture or atoms, often called the "sample", the electron wave would be described in terms of near field or Fresnel diffraction. This has relevance for imaging within electron microscopes, whereas electron diffraction patterns are measured far from the sample, which is described as far-field or Fraunhofer diffraction. A map of the directions of the electron waves leaving the sample will show high intensity (white) for favored directions, such as the three prominent ones in the Young's two-slit experiment of Figure 2, while the other directions will be low intensity (dark). Often there will be an array of spots (preferred directions) as in Figure 1 and the other figures shown later. == History ==
History
The historical background is divided into several subsections. The first is the general background to electrons in vacuum and the technological developments that led to cathode-ray tubes as well as vacuum tubes that dominated early television and electronics; the second is how these led to the development of electron microscopes; the last is work on the nature of electron beams and the fundamentals of how electrons behave, a key component of quantum mechanics and the explanation of electron diffraction. Electrons in vacuum Experiments involving electron beams occurred long before the discovery of the electron; ēlektron (ἤλεκτρον) is the Greek word for amber, which is connected to the recording of electrostatic charging by Thales of Miletus around 585 BCE, and possibly others even earlier. allowing for the study of the effects of high voltage electricity passing through rarefied air. In 1838, Michael Faraday applied a high voltage between two metal electrodes at either end of a glass tube that had been partially evacuated of air, and noticed a strange light arc with its beginning at the cathode (negative electrode) and its end at the anode (positive electrode). Building on this, in the 1850s, Heinrich Geissler was able to achieve a pressure of around 10−3 atmospheres, inventing what became known as Geissler tubes. Using these tubes, while studying electrical conductivity in rarefied gases in 1859, Julius Plücker observed that the radiation emitted from the negatively charged cathode caused phosphorescent light to appear on the tube wall near it, and the region of the phosphorescent light could be moved by application of a magnetic field. In 1869, Plücker's student Johann Wilhelm Hittorf found that a solid body placed between the cathode and the phosphorescence would cast a shadow on the tube wall, e.g. Figure 3. Hittorf inferred that there are straight rays emitted from the cathode and that the phosphorescence was caused by the rays striking the tube walls. In 1876 Eugen Goldstein showed that the rays were emitted perpendicular to the cathode surface, which differentiated them from the incandescent light. Eugen Goldstein dubbed them cathode rays. By the 1870s William Crookes and others were able to evacuate glass tubes below 10−6 atmospheres, and observed that the glow in the tube disappeared when the pressure was reduced but the glass behind the anode began to glow. Crookes was also able to show that the particles in the cathode rays were negatively charged and could be deflected by an electromagnetic field. proving they were made of particles. These particles, however, were 1800 times lighter than the lightest particle known at that time – a hydrogen atom. These were originally called corpuscles and later named electrons by George Johnstone Stoney. The control of electron beams that this work led to resulted in significant technology advances in electronic amplifiers and television displays. introduced his theory of electron waves. He suggested that an electron around a nucleus could be thought of as standing waves, This rapidly became part of what was called by Erwin Schrödinger undulatory mechanics, now called the Schrödinger equation or wave mechanics. As stated by Louis de Broglie on September 8, 1927, in the preface to the German translation of his theses (in turn translated into English): as well as many other phenomena. the other by George Paget Thomson and Alexander Reid; see note for more discussion. Alexander Reid, who was Thomson's graduate student, performed the first experiments, but he died soon after in a motorcycle accident and is rarely mentioned. These experiments were rapidly followed by the first non-relativistic diffraction model for electrons by Hans Bethe diffraction in liquids by Louis Maxwell, and the first electron microscopes developed by Max Knoll and Ernst Ruska. Electron microscopes and early electron diffraction In order to have a practical microscope or diffractometer, just having an electron beam was not enough, it needed to be controlled. Many developments laid the groundwork of electron optics; see the paper by Chester J. Calbick for an overview of the early work. One significant step was the work of Heinrich Hertz in 1883 who made a cathode-ray tube with electrostatic and magnetic deflection, demonstrating manipulation of the direction of an electron beam. Others were focusing of electrons by an axial magnetic field by Emil Wiechert in 1899, improved oxide-coated cathodes which produced more electrons by Arthur Wehnelt in 1905 and the development of the electromagnetic lens in 1926 by Hans Busch. Building an electron microscope involves combining these elements, similar to an optical microscope but with magnetic or electrostatic lenses instead of glass ones. To this day the issue of who invented the transmission electron microscope is controversial, as discussed by Thomas Mulvey Extensive additional information can be found in the articles by Martin Freundlich, Reinhold Rüdenberg and Mulvey. One effort was university based. In 1928, at the Technische Hochschule in Charlottenburg (now Technische Universität Berlin), (Professor of High Voltage Technology and Electrical Installations) appointed Max Knoll to lead a team of researchers to advance research on electron beams and cathode-ray oscilloscopes. The team consisted of several PhD students including Ernst Ruska. In 1931, Max Knoll and Ernst Ruska so did not receive a share of the Nobel Prize in Physics in 1986.) Apparently independent of this effort was work at Siemens-Schuckert by Reinhold Rudenberg. According to patent law (U.S. Patent No. 2058914 and 2070318, both filed in 1932), he is the inventor of the electron microscope, but it is not clear when he had a working instrument. He stated in a very brief article in 1932 that Siemens had been working on this for some years before the patents were filed in 1932, so his effort was parallel to the university effort. He died in 1961, so similar to Max Knoll, was not eligible for a share of the Nobel Prize. These instruments could produce magnified images, but were not particularly useful for electron diffraction; indeed, the wave nature of electrons was not exploited during the development. Key for electron diffraction in microscopes was the advance in 1936 where showed that they could be used as micro-diffraction cameras with an aperture—the birth of selected area electron diffraction. and in 1932 Harrison E. Farnsworth probed single crystals of copper and silver. However, the vacuum systems available at that time were not good enough to properly control the surfaces, and it took almost forty years before these became available. Similarly, it was not until about 1965 that Peter B. Sewell and M. Cohen demonstrated the power of RHEED in a system with a very well controlled vacuum. Subsequent developments in methods and modelling Despite early successes such as the determination of the positions of hydrogen atoms in NH4Cl crystals by W. E. Laschkarew and I. D. Usykin in 1933, boric acid by John M. Cowley in 1953 and orthoboric acid by William Houlder Zachariasen in 1954, electron diffraction for many years was a qualitative technique used to check samples within electron microscopes. John M Cowley explains in a 1968 paper: Thus was founded the belief, amounting in some cases almost to an article of faith, and persisting even to the present day, that it is impossible to interpret the intensities of electron diffraction patterns to gain structural information.This has changed, in transmission, reflection and for low energies. Some of the key developments (some of which are also described later) from the early days to 2023 have been: • Fast numerical methods based upon the Cowley–Moodie multislice algorithm, which only became possible once the fast Fourier transform (FFT) method was developed. With these and other numerical methods Fourier transforms are fast, and it became possible to calculate accurate, dynamical diffraction in seconds to minutes with laptops using widely available multislice programs. • Developments in the convergent-beam electron diffraction approach. Building on the original work of Walther Kossel and Gottfried Möllenstedt in 1939, then mainly by the groups of John Steeds and Michiyoshi Tanaka who showed how to determine point groups and space groups. It can also be used for higher-level refinements of the electron density; for a brief history see CBED history. In many cases this is the best method to determine symmetry. see PED history for further details. Not only is it easier to identify known structures with this approach, it can also be used to solve unknown structures in some cases) to better control surfaces, making LEED and RHEED more reliable and reproducible techniques. In the early days the surfaces were not well controlled; with these technologies they can both be cleaned and remain clean for hours to days, a key component of surface science. and direct electron detectors, which improve the accuracy and reliability of intensity measurements. These have efficiencies and accuracies that can be a thousand or more times that of the photographic film used in the earliest experiments, with the information available in real time rather than requiring photographic processing after the experiment. == Core elements of electron diffraction ==
Core elements of electron diffraction
Plane waves, wavevectors and reciprocal lattice What is seen in an electron diffraction pattern depends upon the sample and also the energy of the electrons. The electrons need to be considered as waves, which involves describing the electron via a wavefunction, written in crystallographic notation (see notes and) as: or probability current which as spin does not normally matter can be reduced to the Klein–Gordon equation. Fortunately one can side-step many complications and use a non-relativistic approach based around the Schrödinger equation. and Archibald Howie, the relationship between the total energy of the electrons and the wavevector is written as:E = \frac{h^2 k^2}{2m^*}withm^* = m_0 + \frac{E}{2c^2}where h is the Planck constant, m^* is a relativistic effective mass used to cancel out the relativistic terms for electrons of energy E with c the speed of light and m_0 the rest mass of the electron. The concept of effective mass occurs throughout physics (see for instance Ashcroft and Mermin), and comes up in the behavior of quasiparticles. A common one is the electron hole, which acts as if it is a particle with a positive charge and a mass similar to that of an electron, although it can be several times lighter or heavier. For electron diffraction the electrons behave as if they are non-relativistic particles of mass m^* in terms of how they interact with the atoms. electron diffraction involves electrons up to . The magnitude of the interaction of the electrons with a material scales as2 \pi \frac{m^*}{h^2 k} = 2\pi\frac{ m^* \lambda} {h^2} = \frac \pi {hc} \sqrt{\frac{2m_0 c^2}{E} + 1}.While the wavevector increases as the energy increases, the change in the effective mass compensates this so even at the very high energies used in electron diffraction there are still significant interactions. Around each reciprocal lattice point one has this shape function. How much intensity there will be in the diffraction pattern depends upon the intersection of the Ewald sphere, that is energy conservation, and the shape function around each reciprocal lattice point—see Figure 6, 20 and 22. The vector from a reciprocal lattice point to the Ewald sphere is called the excitation error \mathbf s_g. For transmission electron diffraction the samples used are thin, so most of the shape function is along the direction of the electron beam. For both LEED For all cases, when the reciprocal lattice points are close to the Ewald sphere (the excitation error is small) the intensity tends to be higher; when they are far away it tends to be smaller. The set of diffraction spots at right angles to the direction of the incident beam are called the zero-order Laue zone (ZOLZ) spots, as shown in Figure 6. One can also have intensities further out from reciprocal lattice points which are in a higher layer. The first of these is called the first order Laue zone (FOLZ); the series is called by the generic name higher order Laue zone (HOLZ). The result is that the electron wave after it has been diffracted can be written as an integral over different plane waves: and further reading). For a perfect crystal the intensity for each diffraction spot \mathbf g is then:I_{g} = \left|\phi(\mathbf k)\right|^2 \propto \left|F_{g}\frac{\sin(\pi t s_z)}{\pi s_z}\right|^2 where s_z is the magnitude of the excitation error |\mathbf s_z| along z, the distance along the beam direction (z-axis by convention) from the diffraction spot to the Ewald sphere, and F_{g} is the structure factor: \mathbf g the reciprocal lattice vector, T_j is a simplified form of the Debye–Waller factor, If a diffraction spot is strong it could be because it has a larger structure factor, or it could be because the combination of thickness and excitation error is "right". Similarly the observed intensity can be small, even though the structure factor is large. This can complicate interpretation of the intensities. By comparison, these effects are much smaller in x-ray diffraction or neutron diffraction because they interact with matter far less and often Bragg's law These are based around solutions of the Schrödinger equation also called an "optical potential". matrix methods which are called Bloch-wave approaches or muffin-tin approaches. With these diffraction spots which are not present in kinematical theory can be present, e.g. • Contributions to the diffraction from elastic strain and crystallographic defects, and also what Jens Lindhard called the string potential. • For transmission electron microscopes effects due to variations in the thickness of the sample and the normal to the surface. and RHEED, Without these the calculations may not be accurate enough. are linear features created by electrons scattered both inelastically and elastically. As the electron beam interacts with matter, the electrons are diffracted via elastic scattering, and also scattered inelastically losing part of their energy. These occur simultaneously, and cannot be separated – according to the Copenhagen interpretation of quantum mechanics, only the probabilities of electrons at detectors can be measured. These electrons form Kikuchi lines which provide information on the orientation. material, within the stereographic triangle|alt=A Kukuchi map, which is a collage of diffraction patterns used to both determine crystal orientation and also to tilt to different orientations. Kikuchi lines come in pairs forming Kikuchi bands, and are indexed in terms of the crystallographic planes they are connected to, with the angular width of the band equal to the magnitude of the corresponding diffraction vector |\mathbf g|. The position of Kikuchi bands is fixed with respect to each other and the orientation of the sample, but not against the diffraction spots or the direction of the incident electron beam. As the crystal is tilted, the bands move on the diffraction pattern. Since the position of Kikuchi bands is quite sensitive to crystal orientation, they can be used to fine-tune a zone-axis orientation or determine crystal orientation. They can also be used for navigation when changing the orientation between zone axes connected by some band, an example of such a map produced by combining many local sets of experimental Kikuchi patterns is in Figure 8; Kikuchi maps are available for many materials. == Types and techniques ==
Types and techniques
In a transmission electron microscope (converging), and ring diffraction (parallel with many grains).|alt=Electron diffraction patterns from different types of crystals and different incident beam convergence. Electron diffraction in a TEM exploits controlled electron beams using electron optics. Different types of diffraction experiments, for instance Figure 9, provide information such as lattice constants, symmetries, and sometimes to solve an unknown crystal structure. It is common to combine it with other methods, for instance images using selected diffraction beams, high-resolution images showing the atomic structure, chemical analysis through energy-dispersive x-ray spectroscopy, investigations of electronic structure and bonding through electron energy loss spectroscopy, and studies of the electrostatic potential through electron holography; this list is not exhaustive. Compared to x-ray crystallography, TEM analysis is significantly more localized and can be used to obtain information from tens of thousands of atoms to just a few or even single atoms. Formation of a diffraction pattern In TEM, the electron beam passes through a thin film of the material as illustrated in Figure 10. Before and after the sample the beam is manipulated by the electron optics these act on the electrons similar to how glass lenses focus and control light. Optical elements above the sample are used to control the incident beam which can range from a wide and parallel beam to one which is a converging cone and can be smaller than an atom, 0.1 nm. As it interacts with the sample, part of the beam is diffracted and part is transmitted without changing its direction. This occurs simultaneously as electrons are everywhere until they are detected (wavefunction collapse) according to the Copenhagen interpretation. Below the sample, the beam is controlled by another set of magnetic lenses and apertures. However, projector lens aberrations such as barrel distortion as well as dynamical diffraction effects (e.g.) cannot be ignored. For instance, certain diffraction spots which are not present in x-ray diffraction can appear, or automated diffraction tomography to solve crystal structures. Polycrystalline pattern using simulation engine of CrysTBox. Corresponding experimental patterns can be seen in Figure 13. |alt=A pattern showing how diffraction patterns from different grain build up to yield a ring pattern. Diffraction patterns depend on whether the beam is diffracted by one single crystal or by a number of differently oriented crystallites, for instance in a polycrystalline material. If there are many contributing crystallites, the diffraction image is a superposition of individual crystal patterns, see Figure 12. With a large number of grains this superposition yields diffraction spots of all possible reciprocal lattice vectors. This results in a pattern of concentric rings as shown in Figure 12 and 13. Here high-resolution transmission electron microscopy and fluctuation electron microscopy can be more powerful, although this is still a topic of continuing development. Multiple materials and double diffraction In simple cases there is only one grain or one type of material in the area used for collecting a diffraction pattern. However, often there is more than one. If they are in different areas then the diffraction pattern will be a combination. • Chemical ordering, that is different atom types at different locations of the subcell. • Magnetic order of the spins. These may be in opposite directions on some atoms, leading to what is called antiferromagnetism. In addition to those which occur in the bulk, superstructures can also occur at surfaces. When half the material is (nominally) removed to create a surface, some of the atoms will be under coordinated. To reduce their energy they can rearrange. Sometimes these rearrangements are relatively small; sometimes they are quite large. Similar to a bulk superstructure there will be additional, weaker diffraction spots. One example is for the silicon (111) surface, where there is a supercell which is seven times larger than the simple bulk cell in two directions. This leads to diffraction patterns with additional spots some of which are marked in Figure 14. Here the (220) are stronger bulk diffraction spots, and the weaker ones due to the surface reconstruction are marked 7 × 7—see note for convention comments. Aperiodic materials In an aperiodic crystal the structure can no longer be simply described by three different vectors in real or reciprocal space. In general there is a substructure describable by three (e.g. \mathbf a, \mathbf b, \mathbf c), similar to supercells above, but in addition there is some additional periodicity (one to three) which cannot be described as a multiple of the three; it is a genuine additional periodicity which is an irrational number relative to the subcell lattice. The diffraction pattern can then only be described by more than three indices. An extreme example of this is for quasicrystals, which can be described similarly by a higher number of Miller indices in reciprocal space—but not by any translational symmetry in real space. An example of this is shown in Figure 15 for an Al–Cu–Fe–Cr decagonal quasicrystal grown by magnetron sputtering on a sodium chloride substrate and then lifted off by dissolving the substrate with water. In the pattern there are pentagons which are a characteristic of the aperiodic nature of these materials. Diffuse scattering A further step beyond superstructures and aperiodic materials is what is called diffuse scattering in electron diffraction patterns due to disorder, or neutron scattering. This can occur from inelastic processes, for instance, in bulk silicon the atomic vibrations (phonons) are more prevalent along specific directions, which leads to streaks in diffraction patterns. Convergent beam electron diffraction In convergent beam electron diffraction (CBED), As illustrated in Figure 18, the details within the disk change with sample thickness, as does the inelastic background. With appropriate analysis CBED patterns can be used for indexation of the crystal point group, space group identification, measurement of lattice parameters, thickness or strain. Precession electron diffraction Precession electron diffraction (PED), invented by Roger Vincent and Paul Midgley in 1994, is a method to collect electron diffraction patterns in a transmission electron microscope (TEM). The technique involves rotating (precessing) a tilted incident electron beam around the central axis of the microscope, compensating for the tilt after the sample so a spot diffraction pattern is formed, similar to a SAED pattern. However, a PED pattern is an integration over a collection of diffraction conditions, see Figure 19. This integration produces a quasi-kinematical diffraction pattern that is more suitable as input into direct methods algorithms using electrons to determine the crystal structure of the sample. Because it avoids many dynamical effects it can also be used to better identify crystallographic phases. 4D STEM 4D scanning transmission electron microscopy (4D STEM) is a subset of scanning transmission electron microscopy (STEM) methods which uses a pixelated electron detector to capture a convergent beam electron diffraction (CBED) pattern at each scan location; see the main page for further information. This technique captures a 2 dimensional reciprocal space image associated with each scan point as the beam rasters across a 2 dimensional region in real space, hence the name 4D STEM. Its development was enabled by better STEM detectors and improvements in computational power. The technique has applications in diffraction contrast imaging, phase orientation and identification, strain mapping, and atomic resolution imaging among others; it has become very popular and rapidly evolving from about 2020 onwards. Most of these are the same, although there are instances such as momentum-resolved STEM where the emphasis can be very different. Low-energy electron diffraction (LEED) Low-energy electron diffraction (LEED) is a technique for the determination of the surface structure of single-crystalline materials by bombardment with a collimated beam of low-energy electrons (30–200 eV). In this case the Ewald sphere leads to approximately back-reflection, as illustrated in Figure 20, and diffracted electrons as spots on a fluorescent screen as shown in Figure 21; see the main page for more information and references. It has been used to solve a very large number of relatively simple surface structures of metals and semiconductors, plus cases with simple chemisorbants. For more complex cases transmission electron diffraction or surface x-ray diffraction have been used, often combined with scanning tunneling microscopy and density functional theory calculations. LEED may be used in one of two ways: is a technique used to characterize the surface of crystalline materials by reflecting electrons off a surface. As illustrated for the Ewald sphere construction in Figure 22, it uses mainly the higher-order Laue zones which have a reflection component. An experimental diffraction pattern is shown in Figure 23 and shows both rings from the higher-order Laue zones and streaky spots. Low-energy electron diffraction (LEED) is also surface sensitive, and achieves surface sensitivity through the use of low energy electrons. The main uses of RHEED to date have been during thin film growth, as the geometry is amenable to simultaneous collection of the diffraction data and deposition. It can, for instance, be used to monitor surface roughness during growth by looking at both the shapes of the streaks in the diffraction pattern as well as variations in the intensities. A gas carrying the molecules is exposed to the electron beam, which is diffracted by the molecules. Since the molecules are randomly oriented, the resulting diffraction pattern consists of broad concentric rings, see Figure 24. The diffraction intensity is a sum of several components such as background, atomic intensity or molecular intensity. I_\text{tot}(s) = I_a(s) + I_m(s) + I_t(s) + I_b(s) ,where I_a(s) results from scattering by individual atoms, I_m(s) by pairs of atoms and I_t(s) by atom triplets. Intensity I_b(s) corresponds to the background which, unlike the previous contributions, must be determined experimentally. The intensity of atomic scattering I_a(s) is defined as I_m(s) = \frac{K^2}{R^2} I_0 \sum_{i=1}^N \sum_{\stackrel{j=1}{i\neq j}}^N \left| f_i(s) \right| \left| f_j(s)\right| \frac{\sin [s(r_{ij}-\kappa s^2)]}{sr_{ij}} e^{-(1/2 l_{ij} s^2)} \cos [\eta _i (s) - \eta _i (s)] ,where r_{ij} is the distance between two atoms, l_{ij} is the mean square amplitude of vibration between the two atoms, similar to a Debye–Waller factor, \kappa is the anharmonicity constant and \eta a phase factor which is important for atomic pairs with very different nuclear charges. The summation is performed over all atom pairs. Atomic triplet intensity I_t(s) is negligible in most cases. If the molecular intensity is extracted from an experimental pattern by subtracting other contributions, it can be used to match and refine a structural model against the experimental data. In a scanning electron microscope .|alt=Kikuchi pattern, a set of line-like features from a scanning electron microscope. In a scanning electron microscope the region near the surface can be mapped using an electron beam that is scanned in a grid across the sample. A diffraction pattern can be recorded using electron backscatter diffraction (EBSD), as illustrated in Figure 25, captured with a camera inside the microscope. A depth from a few nanometers to a few microns, depending upon the electron energy used, is penetrated by the electrons, some of which are diffracted backwards and out of the sample. As result of combined inelastic and elastic scattering, typical features in an EBSD image are Kikuchi lines. Since the position of Kikuchi bands is highly sensitive to the crystal orientation, EBSD data can be used to determine the crystal orientation at particular locations of the sample. The data are processed by software yielding two-dimensional orientation maps. As the Kikuchi lines carry information about the interplanar angles and distances and, therefore, about the crystal structure, they can also be used for phase identification == Notes ==
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