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Focused electron- and ion-beam induced processing are well established techniques for local deposition and etching that rely on decomposition of precursor molecules by irradiation. These high-resolution nanostructuring techniques have various applications in nanoscience including attach-and-release procedures in nanomanipulation and fabrication of sensors (magnetic, optical and thermal) for scanning probe microscopy. However, a complete physical and chemical understanding of the process is hampered by the lack of suitable means to monitor and to access the numerous interrelated and time-varying process parameters (deposition and etch rate, yield, molecule flux and adsorption/desorption). This thesis is a first attempt to fill this gap. It is based on experimental and simulative approaches for the determination of process conditions and mechanical properties of deposited materials: Mass and force sensors: The use of tools merging micromechanical cantilever sensors and scanning electron microscopy was demonstrated for in situ monitoring and analysis. A cantilever-based resonant mass sensing setup was developed and used for real-time mass measurements. A noise level at the femtogram-scale was achieved by tracking the resonance frequency of a temperature stabilized piezoresistive cantilever using phase-locking. With this technique the surface coverage and residence time of (CH3)3PtCpCH3 molecules, the mass deposition rate, the yield, and the material density of corresponding deposits were measured. In situ cantilever-based static force sensing and mechanical modal vibration analysis were employed to investigate the Young's modulus and density of individual high aspect ratio deposits from the precursor Cu(hfac)2. Precursor supply simulations and experiments: A prerequisite to understand and quantify irradiative precursor chemistry is the knowledge of the local flux of molecules impinging on the substrate. Therefore, Monte Carlo simulations of flux distributions were developed and gas flows injected into a vacuum chamber were analyzed experimentally for the precursors Co2(CO)8, (hfac)CuVTMS, and [(PF3)2RhCl]2. The process parameters extracted from the mentioned approaches are valuable input for numerical focused electron- and ion-beam induced process models (Monte Carlo, continuum). We evaluated the precursor surface diffusion coefficient and the electron impact dissociation cross-section by relating deposit shapes to a continuum model.