In this work, a new method for mass determination of single low-charged particles in the sub-picogram regime is developed. It opens applications to chemical physics and surface science via determination of growth rates. The method combines the well-known electrodynamic quadrupole ion trap in a UHV-chamber and fourier transformation of scattered light. The achieved mass resolution of down to $10^{-4}$ at 100 fg mass on a time scale of ten seconds allows a resolution of a few percent of the mass of an adsorbed monolayer and to determine growth rates down to one molecule per second on a time scale of one day. The observation of temperature dependent sticking coefficients results in the measures of the energy of an adsorption barrier. Observation of discrete steps in the rate gives information about the density of molecules in an ordered layer. Temperature dependent desorption data gives the binding energy. The dependence of these observables on the controllable curvature and charge of the substrate's surface is measurable. The first part of this dissertation consists of a description of the common theory of the quadrupole ion trap with the completion of not widely known, newly introduced, contributions to the trapping potential. These contributions lead to systematic shifts in the mass determination. In particular the influence of the inhomogenity of the electrical field, that is used for compensating the gravitational force, is investigated analytically and corroborated experimentally. It is assumed, that the particle's finite size effects in a further shift. In the experimental part initial demonstrative measurements are presented: the time-resolved adsorption of fullerene, anthracene and NO on silica spheres with 500nm diameter has been measured at room temperature. In addition the secondary electron yield of in-situ prepared particles during irradiation with monoenergetic electrons has been determined by analyzing the distribution of change of the number of elementary charges by single events of charging.

A procedure to evaluate the leaching properties of radionuclides from irradiated graphite waste has been developed by combining ANSI 16.1 (USA) and NEN 7345 (Netherlands) standardised diffusion leaching techniques. The ANSI 16.1 standard has been followed to the acquire the leachates and to determine the leach rate/ diffusion coefficient and NEN 7345 standard technique has been used to determine the diffusion mechanism of radionuclides. The investigation employs simulated Drigg groundwater as a leachant using semi-dynamic technique for the production of leachate specimens. From gamma spectroscopy analysis the principal radionuclides present in terms of activity were 60Co, 137Cs, 134Cs, 155Eu, 133Ba and 46Sc. The dominant radionuclides are 60Co, 134Cs and 133Ba which together account for about 91 % of the total activity. The 91 % can be broken down into 73.4 % 60Co, 9.1 % 134Cs and 8.1 % 133Ba. Analysis of total beta and total beta without tritium activity release from Magnox graphite was measured using liquid scintillating counting. Preliminary results show that there is an initial high release of activity and decreases when the leaching period increases. This may be due to the depletion of contaminants which were absorbed by the internal pore networks and the surface. During the leaching test approximately 275.33 ± 18.20 Bq of 3H and 106.26 ± 7.01 Bq of 14C was released into the leachant within 91 days. Irradiation induced damages to the nuclear graphite crystal structure have been shown to cause disruption of the bonding across the basal planes. Moreover, the closures of Mrozowski cracks have been observed in nuclear graphite, the bulk property are governed by the porosity, in particular, at the nanometre scale. Therefore, knowledge of the crystallite structure and porosity distribution is very important; as it will assist in understand the affects of irradiated damage and location and the mechanism of the leaching of radionuclides. The work reported herein contributed several key findings to the international work on graphite leaching to offer guidance leading toward obtaining leaching data in the future: (a) the effective diffusion coefficient for 14C from graphite waste has been determined. The diffusion process for 14C has two stages resulting two different values of diffusion coefficient, i.e., for the fast and slow components; (b) the controlling leaching mechanism for 3H radionuclide from graphite is shown to be surface wash–off; and for that of 14C radionuclide the initial controlling leaching mechanism is surface wash-off following by diffusion which is the major transport mechanism ; (c) The weight loss originates from the open pore structure which has been opened up by radiolytic oxidation; at the higher weight losses much of the closed porosity in the graphite has been opened. The investigation indicates that weigh loss has a major influence on the leaching of elements from the irradiated graphite; and (d) the analysis of the pores in nuclear graphite can be categorised into three types. These three types of pores are: (1) small pores narrow which are slit-shaped pores in the binder phase or matrix, (2) gas evolution pores or gas entrapment pores within the binder phase or matrix and (3) lenticular pores which are large cracks within the filler particles. It is shown in this thesis that by using tomography to study the morphology of the different pores coupled with the distribution of impurities an understanding of the role of porosity in leaching is possible.

This work deal with the analysis of influence of pressure‘s sizes in vacuum chamber of specimen Evironmental Scanning Electron Microscope and the influence of sizes of aperture diaphragm by scintillation detector. The analysis proceeds in detector of secondary electrons. The detector is modelled by system 3D CAD SolidWorks with the help of system CAE Cosmos FloWorks.

The thesis deals with the scintillation secondary electron detector for environmental scanning electron microscope, its design and construction. The starting point was numerical simulation of electrostatic fields and electron trajectories in the electrode system of the detector and simulation of pressure distribution and flow of gases in different parts of the detector. On the basis of modeling and simulation, construction changes of the detector were gradually implemented. Detection efficiency of each version of the detector was determined by the method described in the work. This method enables to evaluate signal level from the captured images of the specimen, quality of images was stated from signal to noise ratio. The thesis describes the whole process of the detector improvement from initial state, when the detector operated with lower efficiency in the pressure range from 300 to 900 Pa, to final version that enables usage of the detector in the range from vacuum up to 1000 Pa of water vapors in the specimen chamber of the microscope.

Thesis deals with theoretical knowledge about scanning electron microscopy and environmental scanning electron microscopy. It describes principle of operation, signals generated by interaction between primary electron beam and specimen and means of detection of secondary electron signal in environmental conditions using scintillation detector. Furthermore, thesis focuses on optimization of detection od secondary electrons by adjusting electrode system of scintillation detector. Computer program Simion is used for modelling signal electron trajectories for proper adjustments. Simulation were starting-point for adjusting the design of the detector. Detection efficiency of adjusted detector was determined by evaluating signal magnitude from captured images, secondary electron detection capability from voltage contrast and quality of the captured images from signal/noise ratio.

In this work, a new method for mass determination of single low-charged particles in the sub-picogram regime is developed. It opens applications to chemical physics and surface science via determination of growth rates. The method combines the well-known electrodynamic quadrupole ion trap in a UHV-chamber and fourier transformation of scattered light. The achieved mass resolution of down to $10^{-4}$ at 100 fg mass on a time scale of ten seconds allows a resolution of a few percent of the mass of an adsorbed monolayer and to determine growth rates down to one molecule per second on a time scale of one day. The observation of temperature dependent sticking coefficients results in the measures of the energy of an adsorption barrier. Observation of discrete steps in the rate gives information about the density of molecules in an ordered layer. Temperature dependent desorption data gives the binding energy. The dependence of these observables on the controllable curvature and charge of the substrate's surface is measurable. The first part of this dissertation consists of a description of the common theory of the quadrupole ion trap with the completion of not widely known, newly introduced, contributions to the trapping potential. These contributions lead to systematic shifts in the mass determination. In particular the influence of the inhomogenity of the electrical field, that is used for compensating the gravitational force, is investigated analytically and corroborated experimentally. It is assumed, that the particle's finite size effects in a further shift. In the experimental part initial demonstrative measurements are presented: the time-resolved adsorption of fullerene, anthracene and NO on silica spheres with 500nm diameter has been measured at room temperature. In addition the secondary electron yield of in-situ prepared particles during irradiation with monoenergetic electrons has been determined by analyzing the distribution of change of the number of elementary charges by single events of charging.

No description available.