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Spontaneous growth of arsenolite micro-crystals at room temperature after high fluence, low energy arsenic trihydride implantation in silicon was observed on the wafer surface after exposure to air. The crystals have been identified unambiguously by x-ray absorption and fluorescence spectroscopy. Thermal treatment easily sublimates the crystals at temperatures as low as 200 °C without any relevant in-diffusion of As into the substrate. The deposition of a thin As-rich layer under high fluence implantation conditions is suggested as possible precursor for crystal formation. The same layer can explain the anomalous retained dose increase often observed after annealing.