Annealing at moderate temperatures is required to activate the silicon surface passivation by Al2O3 thin films while also the thermal stability at higher temperatures is important when Al2O3 is implemented in solar cells with screenprinted metallization. In this paper, the relationship between the microstructure of the Al2O3 film, hydrogen diffusion, and defect passivation is explored in detail for a wide range of annealing temperatures. The chemical passivation was studied using stacks of thermally-grown SiO2 and Al2O3 synthesized by atomic layer deposition. Thermal effusion measurements of hydrogen and implanted He and Ne atoms were used to elucidate the role of hydrogen during annealing. We show that the passivation properties were strongly dependent on the annealing temperature and time and were significantly influenced by the Al2O3 microstructure. The latter was tailored by variation of the deposition temperature (Tdep = 50 °C–400 °C) with hydrogen concentration [H] between 1 and 13 at.% and mass density ρmass between 2.7 and 3.2 g/cm3. In contrast to films with intermediate material properties, the passivation by low- and high density films showed a reduced thermal stability at relatively high annealing temperatures (∼600 °C). These observations proved to be in good agreement with thermal effusion results of hydrogen and inert gas atoms that were also strongly dependent on film microstructure. We demonstrate that the temperature of maximum effusion decreased for films with progressively lower density (i.e., with increasing [H]). Therefore, the reduced thermal stability of the passivation for low-density hydrogen-rich ([H] >∼5 at. %) films can be attributed to a loss of hydrogen at relatively low annealing temperatures. In contrast, the lower initial [H] for dense Al2O3 films can likely explain the lower thermal stability associated with these films. The effusion measurements also allowed us to discuss the role of molecular- and atomic hydrogen during annealing.
The role of hydrogen in Si surface passivation is experimentally identified for Al2O3 (capping) films synthesized by atomic layer deposition. By using stacks of SiO2 and deuterated Al2O3, we demonstrate that hydrogen is transported from Al2O3 to the underlying SiO2 already at relatively low annealing temperatures of 400 °C. This leads to a high level of chemical passivation of the interface. Moreover, the thermal stability of the passivation up to 800 °C was significantly improved by applying a thin Al2O3 capping film on the SiO2. The hydrogen released from the Al2O3 film favorably influences the passivation of Si interface defects.
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Rapid thermal annealing by, e.g., laser scanning of hydrogenated amorphous silicon (a-Si:H) films is of interest for device improvement and for development of new device structures for solar cell and large area display application. For well controlled annealing of such multilayers, precise knowledge of temperature and/or hydrogen diffusion length in the heated material is required but unavailable so far. In this study, we explore the use of deuterium (D) and hydrogen (H) interdiffusion during laser scanning (employing a continuous wave laser at 532 nm wavelength) to characterize both quantities. The evaluation of temperature from hydrogen diffusion data requires knowledge of the high temperature (T > 500 °C) deuterium-hydrogen (D-H) interdiffusion Arrhenius parameters for which, however, no experimental data exist. Using data based on recent model considerations, we find for laser scanning of single films on glass substrates a broad scale agreement with experimental temperature data obtained by measuring the silicon melting point and with calculated data using a physical model as well as published work. Since D-H interdiffusion measures hydrogen diffusion length and temperature within the silicon films by a memory effect, the method is capable of determining both quantities precisely also in multilayer structures, as is demonstrated for films underneath metal contacts. Several applications are discussed. Employing literature data of laser-induced temperature rise, laser scanning is used to measure the H diffusion coefficient at T > 500 °C in a-Si:H. The model-based high temperature hydrogen diffusion parameters are confirmed with important implications for the understanding of hydrogen diffusion in the amorphous silicon material.
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