Heterogeneous Sorption of Radionuclides Predicted by Crystal Surface Nanoroughness

Author(s):  
Tao Yuan ◽  
Stefan Schymura ◽  
Till Bollermann ◽  
Konrad Molodtsov ◽  
Paul Chekhonin ◽  
...  
Keyword(s):  
Author(s):  
G. Lehmpfuhl

Introduction In electron microscopic investigations of crystalline specimens the direct observation of the electron diffraction pattern gives additional information about the specimen. The quality of this information depends on the quality of the crystals or the crystal area contributing to the diffraction pattern. By selected area diffraction in a conventional electron microscope, specimen areas as small as 1 µ in diameter can be investigated. It is well known that crystal areas of that size which must be thin enough (in the order of 1000 Å) for electron microscopic investigations are normally somewhat distorted by bending, or they are not homogeneous. Furthermore, the crystal surface is not well defined over such a large area. These are facts which cause reduction of information in the diffraction pattern. The intensity of a diffraction spot, for example, depends on the crystal thickness. If the thickness is not uniform over the investigated area, one observes an averaged intensity, so that the intensity distribution in the diffraction pattern cannot be used for an analysis unless additional information is available.


Author(s):  
Douglas L. Dorset ◽  
Anthony J. Hancock

Lipids containing long polymethylene chains were among the first compounds subjected to electron diffraction structure analysis. It was only recently realized, however, that various distortions of thin lipid microcrystal plates, e.g. bends, polar group and methyl end plane disorders, etc. (1-3), restrict coherent scattering to the methylene subcell alone, particularly if undistorted molecular layers have well-defined end planes. Thus, ab initio crystal structure determination on a given single uncharacterized natural lipid using electron diffraction data can only hope to identify the subcell packing and the chain axis orientation with respect to the crystal surface. In lipids based on glycerol, for example, conformations of long chains and polar groups about the C-C bonds of this moiety still would remain unknown.One possible means of surmounting this difficulty is to investigate structural analogs of the material of interest in conjunction with the natural compound itself. Suitable analogs to the glycerol lipids are compounds based on the three configurational isomers of cyclopentane-1,2,3-triol shown in Fig. 1, in which three rotameric forms of the natural glycerol derivatives are fixed by the ring structure (4-7).


Author(s):  
G. G. Hembree ◽  
M. A. Otooni ◽  
J. M. Cowley

The formation of oxide structures on single crystal films of metals has been investigated using the REMEDIE system (for Reflection Electron Microscopy and Electron Diffraction at Intermediate Energies) (1). Using this instrument scanning images can be obtained with a 5 to 15keV incident electron beam by collecting either secondary or diffracted electrons from the crystal surface (2). It is particularly suited to studies of the present sort where the surface reactions are strongly related to surface morphology and crystal defects and the growth of reaction products is inhomogeneous and not adequately described in terms of a single parameter. Observation of the samples has also been made by reflection electron diffraction, reflection electron microscopy and replication techniques in a JEM-100B electron microscope.A thin single crystal film of copper, epitaxially grown on NaCl of (100) orientation, was repositioned on a large copper single crystal of (111) orientation.


Author(s):  
H. Hashimoto ◽  
Y. Sugimoto ◽  
Y. Takai ◽  
H. Endoh

As was demonstrated by the present authors that atomic structure of simple crystal can be photographed by the conventional 100 kV electron microscope adjusted at “aberration free focus (AFF)” condition. In order to operate the microscope at AFF condition effectively, highly stabilized electron beams with small energy spread and small beam divergence are necessary. In the present observation, a 120 kV electron microscope with LaB6 electron gun was used. The most of the images were taken with the direct electron optical magnification of 1.3 million times and then magnified photographically.1. Twist boundary of ZnSFig. 1 is the image of wurtzite single crystal with twist boundary grown on the surface of zinc crystal by the reaction of sulphur vapour of 1540 Torr at 500°C. Crystal surface is parallel to (00.1) plane and electron beam is incident along the axis normal to the crystal surface. In the twist boundary there is a dislocation net work between two perfect crystals with a certain rotation angle.


Author(s):  
S. Kimoto ◽  
H. Hashimoto ◽  
S. Takashima ◽  
R. M. Stern ◽  
T. Ichinokawa

The most well known application of the scanning microscope to the crystals is known as Coates pattern. The contrast of this image depends on the variation of the incident angle of the beam to the crystal surface. The defect in the crystal surface causes to make contrast in normal scanning image with constant incident angle. The intensity variation of the backscattered electrons in the scanning microscopy was calculated for the defect in the crystals by Clarke and Howie. Clarke also observed the defect using a scanning microscope.This paper reports the observation of lattice defects appears in thin crystals through backscattered, secondary and transmitted electron image. As a backscattered electron detector, a p-n junction detector of 0.9 π solid angle has been prepared for JSM-50A. The gain of the detector itself is 1.2 x 104 at 50 kV and the gain of additional AC amplifier using band width 100 Hz ∼ 10 kHz is 106.


Author(s):  
M. Pan ◽  
J.M. Cowley

Electron microdiffraction patterns, obtained when a small electron probe with diameter of 10-15 Å is directed to run parallel to and outside a flat crystal surface, are sensitive to the surface nature of the crystals. Dynamical diffraction calculations have shown that most of the experimental observations for a flat (100) face of a MgO crystal, such as the streaking of the central spot in the surface normal direction and (100)-type forbidden reflections etc., could be explained satisfactorily by assuming a modified image potential field outside the crystal surface. However the origin of this extended surface potential remains uncertain. A theoretical analysis by Howie et al suggests that the surface image potential should have a form different from above-mentioned image potential and also be smaller by several orders of magnitude. Nevertheless the surface potential distribution may in practice be modified in various ways, such as by the adsorption of a monolayer of gas molecules.


Author(s):  
R. L. Hines

The importance of atom layer terraces or steps on platinum surfaces used for catalysis as discussed by Somorjai justifies an extensive investigation of the structure of platinum surfaces through electron microscopy at the atomic resolution level. Experimental and theoretical difficulties complicate the quantitative determination of platinum surface structures but qualitative observation of surface structures on platinum crystals is now possible with good experimental facilities.Ultrathin platinum crystals with nominal 111 orientation are prepared using the procedure reported by Hines without the application of a carbon backing layer. Platinum films with thicknesses of about ten atom layers are strong enough so that they can be mounted on grids to provide ultrathin platinum crystals for examination of surface structure. Crystals as thin as possible are desired to minimize the theoretical difficulties in analyzing image contrast to determine structure. With the current preparation procedures the crystals frequently cover complete openings on a 400 mesh grid.


Author(s):  
H.-J. Ou ◽  
J. M. Cowley ◽  
A. A. Higgs

A scanning ion gun system has been installed on the specimen preparation chamber (pressure ∼5xl0-8 torr) of the VG-HB5 STEM microscope. By using the specimen current imaging technique, it is possible to use an ion beam to sputter-clean the preferred surface region on a bulk sample. As shown in figure 1, the X-Y raster-gate control of the scanning unit for the Krato Mini-Beam I is used to minimize the beam raster area down to a 800μm x800μm square region. With beam energy of 2.5KeV, the MgO cleavage surface has been ion sputter-cleaned for less than 1 minute. The carbon film or other contaminant, introduced during the cleavage process in air, is mostly removed from the MgO crystal surfaces.The immediate SREM inspection of this as-cleaned MgO surface, within the adjacent STEM microscope, has revealed the detailed surface structures of atomic steps, which were difficult to observe on the as-cleaved MgO surfaces in the previous studies.


Author(s):  
G. L. Kellogg ◽  
P. R. Schwoebel

Although no longer unique in its ability to resolve individual single atoms on surfaces, the field ion microscope remains a powerful tool for the quantitative characterization of atomic processes on single-crystal surfaces. Investigations of single-atom surface diffusion, adatom-adatom interactions, surface reconstructions, cluster nucleation and growth, and a variety of surface chemical reactions have provided new insights to the atomic nature of surfaces. Moreover, the ability to determine the chemical identity of selected atoms seen in the field ion microscope image by atom-probe mass spectroscopy has increased or even changed our understanding of solid-state-reaction processes such as ordering, clustering, precipitation and segregation in alloys. This presentation focuses on the operational principles of the field-ion microscope and atom-probe mass spectrometer and some very recent applications of the field ion microscope to the nucleation and growth of metal clusters on metal surfaces.The structure assumed by clusters of atoms on a single-crystal surface yields fundamental information on the adatom-adatom interactions important in crystal growth. It was discovered in previous investigations with the field ion microscope that, contrary to intuition, the initial structure of clusters of Pt, Pd, Ir and Ni atoms on W(110) is a linear chain oriented in the <111> direction of the substrate.


Author(s):  
H. Banzhof ◽  
I. Daberkow

A Philips EM 420 electron microscope equipped with a field emission gun and an external STEM unit was used to compare images of single crystal surfaces taken by conventional reflection electron microscopy (REM) and scanning reflection electron microscopy (SREM). In addition an angle-resolving detector system developed by Daberkow and Herrmann was used to record SREM images with the detector shape adjusted to different details of the convergent beam reflection high energy electron diffraction (CBRHEED) pattern.Platinum single crystal spheres with smooth facets, prepared by melting a thin Pt wire in an oxyhydrogen flame, served as objects. Fig. 1 gives a conventional REM image of a (111)Pt single crystal surface, while Fig. 2 shows a SREM record of the same area. Both images were taken with the (555) reflection near the azimuth. A comparison shows that the contrast effects of atomic steps are similar for both techniques, although the depth of focus of the SREM image is reduced as a result of the large illuminating aperture. But differences are observed at the lengthened images of small depressions and protrusions formed by atomic steps, which give a symmetrical contrast profile in the REM image, while an asymmetric black-white contrast is observed in the SREM micrograph. Furthermore the irregular structures which may be seen in the middle of Fig. 2 are not visible in the REM image, although it was taken after the SREM record.


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